Antireflection film and exposure method

ABSTRACT

An antireflection film wherein, even where exposure light enters obliquely in a liquid immersion lithography technique, a sufficiently reduced reflectance can be achieved at the interface between a resist layer and a silicon substrate. A two-layer antireflection film is used in exposure by an exposure system having a wavelength of 190 to 195 nm and a numerical aperture of 1.0 or less and formed between the resist layer and the silicon substrate. Where complex refractive indices N 1  and N 2  and film thicknesses of upper and lower layers of the antireflection film are represented by n 1 -k 1 i, n 2 -k 2 i and d 1 , d 2 , respectively, and a predetermined combination of values of [n 10 , k 10 , d 10 , n 20 , k 20 , d 20 ] is selected, n 1 , k 1 , d 1 , n 2 , k 2  and d 2  satisfy {(n 1 -n 10 )/(n 1m -n 10 )} 2 +{(k 1 -k 10 )/(k 1m -k 10 )} 2 +{(d 1 -d 10 )/(d 1m -d 10 )} 2 +{(n 2 -n 20 )/(n 2m -n 20 )} 2 +{(k 2 -k 20 )/(k 2m -k 20 )} 2 +{(d 2 -d 20 )/(d 2m -d 20 )} 2 ≦1.

CROSS REFERENCES TO RELATED APPLICATIONS

The present invention contains subject matter related to Japanese Patent Application JP 2005-054202 filed in the Japanese Patent Office on Feb. 28, 2005, the entire contents of which being incorporated herein by reference.

BACKGROUND OF THE INVENTION

This invention relates to an antireflection film which is used for exposure of a resist film in a fabrication process of a semiconductor device and an exposure-method in which an antireflection film is used.

In the field of semiconductor devices, together with the advancement of high integration of semiconductor devices, it has become a pressing need to establish a new process technique which permits working of very fine patterns of, for example, 65 nm or less. For the working of fine patterns, a photolithography technique is required essentially. The photolithography technique at present uses an argon-fluorine (ArF) excimer laser of the wavelength of 193 nm as an exposure light source in order to assure an enhanced optical resolution thanks to a reduced wavelength of exposure light (illumination light) so as to be ready for very fine working.

A silicon semiconductor substrate is patterned usually using a photosensitive resist layer formed by coating on the surface of the silicon semiconductor substrate. However, where the reflectance of exposure light (illumination light) at the interface between the resist layer and the silicon semiconductor substrate which serves as a substrate for the resist layer is high, a standing wave is induced conspicuously in the resist layer. As a result, side faces of the resist layer patterned by development exhibit a concave and convex shape in accordance with the shape of the standing wave. Therefore, there is a problem that a pattern of a good rectangular shape cannot be formed on the resist layer. It is to be noted that a pattern formed on a resist layer is sometimes called resist pattern. For example, the reflectance where a resist layer having a refractive index of 1.70 is formed on the surface of a silicon semiconductor substrate using exposure light of a wavelength of 193 nm is a very high value of approximately 60% where the exposure light is incident perpendicularly to the resist layer.

In order to solve such a problem as described above, according to a conventional photolithography technique wherein exposure light of a wavelength of 193 nm is used, an antireflection film of a single layer is formed between the silicon semiconductor substrate and the resist layer. For example, where the complex refractive index is represented by N₀ (where N₀=n₀-k₀i), if an antireflection film of a thickness of 100 nm having such values as n₀=1.75 and k₀=0.30 is formed on the silicon semiconductor substrate and a resist layer having a refractive index of 1.70 is formed on the antireflection film, then the reflectance is reduced by a great amount to approximately 2% where the exposure light is incident perpendicularly to the resist layer.

A related technique is disclosed, for example, in Japanese Patent Laid-open No. 2001-242630 (hereinafter referred to as Patent Document 1) or Boontarika, Ozawa and Someya, Extended Abstracts (The 65th Meeting2004); The Japan Society of Applied Physics, 2p-R-9 (hereinafter referred to as Non-Patent Document 1).

SUMMARY OF THE INVENTION

Incidentally, the critical resolution in the photography technique is approximately equal to 0.3 times the wavelength of exposure light. Accordingly, in a photolithography technique wherein an ArF excimer laser of a wavelength of 193 nm is used as an exposure light source, the critical resolution is approximately 60 nm.

Thus, development of a liquid immersion lithography technique which achieves a further high resolution is being proceeded as a technique for forming a pattern finer than approximately 60 nm on a silicon semiconductor substrate. According to the liquid immersion lithography technique, a medium having a refractive index higher than that of air (for example, immersion liquid formed from water) is filled between an exposure system (illumination system) and a resist layer.

Since the exposure is performed through the immersion liquid, the effective wavelength of the exposure light becomes equal to a value obtained by dividing the wavelength of the exposure light in the vacuum by the refractive index of the immersion liquid, and a higher resolution performance can be achieved. For example, where an ArF excimer laser of a wavelength of 193 nm is used as the exposure light source and water (whose refractive index at the wavelength of 193 nm is 1.44) is used as the immersion liquid, the effective wavelength is approximately 134 nm, and the critical resolution is obtained by multiplying the effective wavelength by 0.3 and is approximately 40 nm. In other words, the liquid immersion lithography wherein water is used allows formation of a pattern finer than approximately 60 nm to be formed on a silicon semiconductor substrate.

Meanwhile, the focus tolerance, i.e., depth of focus (DOF), upon exposure is given by the following expression: DOF=n _(Liq) ·K ₂ ·λ/NA ² where n_(Liq) is the refractive index of the immersion liquid, K₂ a constant which relies upon the process, λ the wavelength of exposure light (illumination light) in the vacuum, and NA the numerical aperture of the exposure system (illumination system).

Accordingly, where the numerical aperture NA is fixed, the focus tolerance DOF in the liquid immersion lithography technique is equal to n_(Liq) times that in the conventional photolithography technique which relies upon exposure in air. In other words, in the liquid immersion lithography technique wherein water is used as the immersion liquid, the focus tolerance DOF increases to 1.44 times. Therefore, a mass production process having a greater margin can be constructed.

However, such a liquid immersion lithography technique as described above has a problem that the single layer antireflection film in the prior art does not function effectively.

Exposure light is transmitted through an incidence medium and enters the resist layer and further enters the antireflection film. Where the incident angle when the exposure light enters the resist layer from the incidence medium is represented by θ_(in), the refractive index of the incidence medium by n_(in), the incident angle when the exposure light enters the silicon semiconductor substrate or the antireflection film from the resist layer by θ_(IF) and the refractive index of a resist material which forms the resist layer by n_(Res), the following expression is satisfied: NA=n _(in)·sin(θ_(in))=n _(Res)·sin(θ_(IF)) It is to be noted that, in the conventional photolithography technique, since the incidence medium is air, the refractive index n_(in) is n_(in)=1, but in the liquid immersion lithography, for example, where water is used as the immersion liquid, since the incidence medium is water, the refractive index n_(in) is n_(in)=1.44.

From the expression above, it can be recognized that, where θ_(in) is fixed, the numerical aperture NA according to the liquid immersion lithography technique increases to n_(Liq) times that according to the conventional photolithography technique (n_(in)=1.0). In other words, if the refractive index n_(Res) of the resist material from which the resist layer is formed is fixed, then sin(θ_(IF)) increases. This signifies that θ_(IF) increases with the liquid immersion lithography technique. In other words, it is considered that, according to the liquid immersion lithography technique, the exposure light enters in a more oblique direction when compared with that according to the conventional photolithography technique.

On the other hand, where an antireflection film of a single layer is used, the reflectance when exposure light enters perpendicularly can be decreased sufficiently. However, there is a problem that the reflectance in oblique incidence of exposure light cannot be reduced sufficiently.

Where an antireflection film of a thickness of 100 nm having a complex reflectance N₀ having such values as n₀=1.75 and k₀=0.30 is formed on the surface of a silicon semiconductor substrate and a resist layer having a refractive index of 1.70 is formed on the antireflection film, the reflectance where the exposure light enters perpendicularly (that is, the incident angle θ_(IF)=0 degree) decreases significantly to approximately 2%. Accordingly, where the incident angle θ_(IF) increases to 55 degrees, the reflectance increases much to approximately 7%.

Meanwhile, as a result of the progress of refinement, the maximum tolerance to the reflectance at the interface between the resist layer and the silicon semiconductor substrate has decreased year by year, and particularly the maximum tolerance to the reflectance in such a fine generation as that wherein a liquid immersion lithography technique is applied is as low as 0.4% as disclosed in Non-Patent Document 1.

In particular, an antireflection film of a single layer used in the conventional photolithography technique cannot reduce the reflectance sufficiently in the liquid immersion lithography technique also because the exposure light enters further obliquely. Further, since the reflectance cannot be reduced sufficiently, the problem that a good rectangular pattern cannot be formed on the resist layer cannot be solved because a standing wave appears significantly in the resist layer.

Accordingly, it is desirable for the present invention to provide an antireflection film wherein, even where exposure light (illumination light) enters a resist layer obliquely in a photolithography technique such as a liquid immersion lithography technique wherein an exposure system (illumination system) has an increased numerical aperture to achieve an increased focus tolerance, a sufficiently reduced reflectance can be achieved at the interface between the resist layer and a silicon semiconductor substrate and an exposure method which uses the antireflection film.

In order to attain the desire described above, according to a first embodiment of the present invention, there is provided an antireflection film having a two-layer structure and formed between a resist layer and a surface of a silicon semiconductor substrate for being used when the resist layer is exposed by an exposure system which is used in a fabrication process of a semiconductor device and has a wavelength of 190 nm to 195 nm and a numerical aperture equal to or less than 1.0. Further, according to the first embodiment of the present invention, there is provided an exposure method for exposing a resist layer by means of an exposure system which is used in a fabrication process of a semiconductor device and has a wavelength of 190 nm to 195 nm and a numerical aperture equal to or less than 1.0, an antireflection film which has a two-layer structure being formed between the resist layer and a surface of a silicon semiconductor substrate.

The antireflection film and the exposure method according to the first embodiment are configured such that the antireflection film includes an upper layer having a complex refractive index N₁ equal to n₁-k₁i and a film thickness d₁ whose unit is nm, and a lower layer having a complex refractive index N₂ equal to n₂-k₂i and a film thickness d₂ whose unit is nm, the upper layer and the lower layer being configured such that, when one of cases [1-01] to [1-16] defined in a table given below is selected as a combination of values of [n₁₀, k₁₀, d₁₀, n₂₀, k₂₀, d₂₀], n₁, k₁, d₁, n₂, k₂ and d₂ satisfy an expression {(n ₁-n ₁₀)/(n _(1m)-n ₁₀)}²+{(k ₁-k ₁₀)/(k _(1m)-k ₁₀)}²+{(d ₁-d ₁₀)/(d _(1m)-d ₁₀)}²+{(n ₂-n ₂₀)/(n _(2m)-n ₂₀)}²+{(k ₂-k ₂₀) /(k _(2m)-k ₂₀)}²+{(d ₂-d ₂₀)/(d _(2m)-d ₂₀)}²≦1 where a value of n_(1m) in the pertaining case is adopted between on a relationship in magnitude between n₁ and n₁₀, a value of k_(1m) in the pertaining case is adopted between on a relationship in magnitude between k₁ and k₁₀, a value of d_(1m) in the pertaining case is adopted between on a relationship in magnitude between d₁ and d₁₀, a value of n_(2m) in the pertaining case is adopted between on a relationship in magnitude between n₂ and n₂₀, a value of k_(2m) in the pertaining case is adopted between on a relationship in magnitude between k₂ and k₂₀, and a value of d_(2m) in the pertaining case is adopted between on a relationship in magnitude between d₂ and d₂₀.

Case 1-01 1-02 1-03 1-04 1-05 n₁₀ 2.1616 1.9575 1.8783 1.8886 1.7671 k₁₀ 0.0031 0.1578 0.1120 0.0828 0.0972 d₁₀(nm) 16.39 29.70 22.79 17.43 89.65 n₂₀ 2.3326 3.1421 1.9535 1.8540 1.7266 k₂₀ 0.9955 0.5540 0.3987 0.3157 0.6265 d₂₀(nm) 21.81 39.99 133.42 201.01 35.79 for n₁ ≧ n₁₀, n_(1m) = 2.2660 2.0526 1.9695 1.9914 1.8452 for n₁ < n₁₀, n_(1m) = 2.0674 1.8816 1.8041 1.8047 1.7221 for k₁ ≧ k₁₀, k_(1m) = 0.1058 0.2476 0.1956 0.1790 0.1791 for k₁ < k₁₀, k_(1m) = 0.0000 0.0772 0.0266 0.0000 0.0475 for d₁ ≧ d₁₀, d_(1m)(nm) = 19.64 35.17 31.59 26.35 108.00 for d₁ < d₁₀, d_(1m)(nm) = 13.49 25.28 16.46 11.04 81.48 for n₂ ≧ n₂₀, n_(2m) = 2.4717 3.2954 2.1133 2.0045 1.8644 for n₂ < n₂₀, n_(2m) = 2.1929 2.9698 1.7768 1.6777 1.5730 for k₂ ≧ k₂₀, k_(2m) = 1.1482 0.7497 0.6196 0.4975 0.7644 for k₂ < k₂₀, k_(2m) = 0.8579 0.4177 0.2781 0.2069 0.4915 for d₂ ≧ d₂₀, d_(2m)(nm) = 25.55 42.99 ∞ ∞ 43.06 for d₂ < d₂₀, d_(2m)(nm) = 18.70 37.27 75.37 118.11 29.14 Case 1-06 1-07 1-08 1-09 1-10 n₁₀ 1.7783 1.7756 1.7637 1.7297 1.7402 k₁₀ 0.0854 0.0827 0.0788 0.0695 0.0705 d₁₀(nm) 90.09 89.16 88.60 159.09 157.00 n₂₀ 1.9451 1.8813 1.8074 1.8027 1.9115 k₂₀ 0.4110 0.2980 0.2358 0.6176 0.3647 d₂₀(nm) 78.70 136.86 201.53 30.94 79.38 for n₁ ≧ n₁₀, n_(1m) = 1.8547 1.8491 1.8363 1.8086 1.8145 for n₁ < n₁₀, n_(1m) = 1.7290 1.7286 1.7192 1.6900 1.6996 for k₁ ≧ k₁₀, k_(1m) = 0.1675 0.1627 0.1158 0.1537 0.1529 for k₁ < k₁₀, k_(1m) = 0.0321 0.0280 0.0215 0.0304 0.0296 for d₁ ≧ d₁₀, d_(1m)(nm) = 108.98 109.36 112.80 ∞ 193.81 for d₁ < d₁₀, d_(1m)(nm) = 80.83 80.19 79.23 146.42 145.32 for n₂ ≧ n₂₀, n_(2m) = 2.0858 2.0287 1.9635 1.9536 2.0439 for n₂ < n₂₀, n_(2m) = 1.7991 1.7335 1.6573 1.6453 1.7648 for k₂ ≧ k₂₀, k_(2m) = 0.5849 0.5031 0.4587 0.7451 0.5149 for k₂ < k₂₀, k_(2m) = 0.2966 0.2049 0.1553 0.4826 0.2558 for d₂ ≧ d₂₀, d_(2m)(nm) = 90.20 ∞ ∞ 36.88 89.13 for d₂ < d₂₀, d_(2m)(nm) = 68.53 118.11 131.91 25.32 69.56 Case 1-11 1-12 1-13 1-14 1-15 n₁₀ 1.7416 1.7346 1.7204 1.7293 1.7290 k₁₀ 0.0723 0.0700 0.0573 0.0638 0.0672 d₁₀(nm) 154.81 154.48 226.55 221.51 219.00 n₂₀ 1.8276 1.7635 1.9505 1.9167 1.7992 k₂₀ 0.2602 0.2082 0.6496 0.3426 0.2416 d₂₀(nm) 140.99 205.63 25.08 78.00 142.68 for n₁ ≧ n₁₀, n_(1m) = 1.8128 1.8044 1.8037 1.8053 1.8030 for n₁ < n₁₀, n_(1m) = 1.7051 1.7002 1.6700 1.6857 1.6894 for k₁ ≧ k₁₀, k_(1m) = 0.1493 0.1428 0.1449 0.1450 0.1411 for k₁ < k₁₀, k_(1m) = 0.0310 0.0277 0.0218 0.0296 0.0354 for d₁ ≧ d₁₀, d_(1m)(nm) = 194.11 ∞ ∞ ∞ ∞ for d₁ < d₁₀, d_(1m)(nm) = 144.88 144.10 147.03 206.52 206.86 for n₂ ≧ n₂₀, n_(2m) = 1.9727 1.9440 2.1270 2.0463 1.9388 for n₂ < n₂₀, n_(2m) = 1.6802 1.6149 1.7784 1.7598 1.6376 for k₂ ≧ k₂₀, k_(2m) = 0.1493 0.4167 0.7867 0.4807 0.4185 for k₂ < k₂₀, k_(2m) = 0.0310 0.1340 0.4991 0.2325 0.1559 for d₂ ≧ d₂₀, d_(2m)(nm) = ∞ ∞ 30.06 87.34 ∞ for d₂ < d₂₀, d_(2m)(nm) = 126.07 175.09 20.53 70.06 130.30 Case 1-16 n₁₀ 1.7210 k₁₀ 0.0630 d₁₀(nm) 220.18 n₂₀ 1.7329 k₂₀ 0.1973 d₂₀(nm) 207.16 for n₁ ≧ n₁₀, n_(1m) = 1.7917 for n₁ < n₁₀, n_(1m) = 1.6626 for k₁ ≧ k₁₀, k_(1m) = 0.1377 for k₁ < k₁₀, k_(1m) = 0.0303 for d₁ ≧ d₁₀, d_(1m)(nm) = ∞ for d₁ < d₁₀, d_(1m)(nm) = 147.71 for n₂ ≧ n₂₀, n_(2m) = 1.9597 for n₂ < n₂₀, n_(2m) = 1.5656 for k₂ ≧ k₂₀, k_(2m) = 0.3989 for k₂ < k₂₀, k_(2m) = 0.1211 for d₂ ≧ d₂₀, d_(2m)(nm) = ∞ for d₂ < d₂₀, d_(2m)(nm) = 174.03

According to a second embodiment of the present invention, there is provided an antireflection film having a two-layer structure and formed between a resist layer and a surface of a silicon semiconductor substrate for being used when the resist layer is exposed by an exposure system which is used in a fabrication process of a semiconductor device and has a wavelength of 190 nm to 195 nm and a numerical aperture more than 1.0 but equal to or less than 1.1. Further, according to the second embodiment of the present invention, there is provided an exposure method for exposing a resist layer by means of an exposure system which is used in a fabrication process of a semiconductor device and has a wavelength of 190 nm to 195 nm and a numerical aperture more than 1.0 but equal to or less than 1.1, an antireflection film which has a two-layer structure being formed between the resist layer and a surface of a silicon semiconductor substrate.

The antireflection film and the exposure method according to the second embodiment are configured such that an upper layer having a complex refractive index N₁ equal to n₁-k₁i and a film thickness d₁ whose unit is nm, and a lower layer having a complex refractive index N₂ equal to n₂-k₂i and a film thickness d₂ whose unit is nm, the upper layer and the lower layer being configured such that, when one of cases [2-01] to [2-16] defined in a table given below is selected as a combination of values of [n₁₀, k₁₀, d₁₀, n₂₀, k₂₀, d₂₀], n₁, k₁, d₁, n₂, k₂ and d₂ satisfy an expression {(n ₁-n ₁₀)/(n _(1m)-n ₁₀)}²+{(k ₁-k ₁₀)/(k _(1m)-k ₁₀)}²+{(d ₁-d ₁₀)/(d _(1m)-d ₁₀)}²+{(n ₂-n ₂₀)/(n _(2m)-n ₂₀)}²+{(k ₂-k ₂₀) /(k _(2m)-k ₂₀)}²+{(d ₂-d ₂₀)/(d _(2m)-d ₂₀)}²≦1 where a value of n_(1m) in the pertaining case is adopted between on a relationship in magnitude between n₁ and n₁₀, a value of k_(1m) in the pertaining case is adopted between on a relationship in magnitude between k₁ and k₁₀, a value of d_(1m) in the pertaining case is adopted between on a relationship in magnitude between d₁ and d₁₀, a value of n_(2m) in the pertaining case is adopted between on a relationship in magnitude between n₂ and n₂₀, a value of k_(2m) in the pertaining case is adopted between on a relationship in magnitude between k₂ and k₂₀, and a value of d_(2m) in the pertaining case is adopted between on a relationship in magnitude between d₂ and d₂₀.

Case 2-01 2-02 2-03 2-04 2-05 n₁₀ 2.1270 1.9689 1.8874 1.9059 1.7643 k₁₀ 0.0000 0.1461 0.1027 0.0744 0.0947 d₁₀(nm) 17.47 29.67 21.38 15.49 94.08 n₂₀ 2.3628 3.1616 1.9199 1.8297 1.7955 k₂₀ 0.9776 0.5440 0.3802 0.2998 0.6320 d₂₀(nm) 21.04 39.98 139.31 207.65 32.98 for n₁ ≧ n₁₀, n_(1m) = 2.2256 2.0568 1.9734 2.0082 1.8353 for n₁ < n₁₀, n_(1m) = 2.0472 1.9010 1.8223 1.8296 1.7330 for k₁ ≧ k₁₀, k_(1m) = 0.0938 0.2244 0.1768 0.1635 0.1575 for k₁ < k₁₀, k_(1m) = 0.0000 0.0685 0.0175 0.0000 0.0495 for d₁ ≧ d₁₀, d_(1m)(nm) = 20.80 34.77 29.62 23.26 112.91 for d₁ < d₁₀, d_(1m)(nm) = 14.63 25.76 16.06 10.49 87.82 for n₂ ≧ n₂₀, n_(2m) = 2.4916 3.3028 2.0581 1.9623 1.9074 for n₂ < n₂₀, n_(2m) = 2.2319 3.0031 1.7577 1.6665 1.6538 for k₂ ≧ k₂₀, k_(2m) = 1.1151 0.7242 0.5735 0.4524 0.7450 for k₂ < k₂₀, k_(2m) = 0.8400 0.4156 0.2710 0.2013 0.5085 for d₂ ≧ d₂₀, d_(2m)(nm) = 24.36 42.69 ∞ ∞ 38.62 for d₂ < d₂₀, d_(2m)(nm) = 18.21 37.46 80.09 126.81 27.34 Case 2-06 2-07 2-08 2-09 2-10 n₁₀ 1.7803 1.7743 1.7445 1.7294 1.7425 k₁₀ 0.0868 0.0850 0.0789 0.0717 0.0762 d₁₀(nm) 93.23 91.77 92.02 166.39 161.95 n₂₀ 1.9791 1.8636 1.7368 1.9163 1.9299 k₂₀ 0.3951 0.2810 0.2206 0.6369 0.3467 d₂₀(nm) 77.05 139.87 212.33 26.72 78.23 for n₁ ≧ n₁₀, n_(1m) = 1.8462 1.8349 1.8028 1.8016 1.8041 for n₁ < n₁₀, n_(1m) = 1.7475 1.7473 1.7193 1.7039 1.7237 for k₁ ≧ k₁₀, k_(1m) = 0.1496 0.1408 0.1323 0.1330 0.1299 for k₁ < k₁₀, k_(1m) = 0.0394 0.0374 0.0301 0.0370 0.0455 for d₁ ≧ d₁₀, d_(1m)(nm) = 109.31 108.27 115.67 209.20 195.88 for d₁ < d₁₀, d_(1m)(nm) = 87.00 86.56 85.73 157.85 156.76 for n₂ ≧ n₂₀, n_(2m) = 2.1009 1.9987 1.8971 2.0476 2.0364 for n₂ < n₂₀, n_(2m) = 1.8504 1.7392 1.6175 1.7703 1.8051 for k₂ ≧ k₂₀, k_(2m) = 0.5318 0.4468 0.3623 0.7342 0.4294 for k₂ < k₂₀, k_(2m) = 0.2922 0.2015 0.1499 0.5070 0.2516 for d₂ ≧ d₂₀, d_(2m)(nm) = 85.43 ∞ ∞ 31.20 85.58 for d₂ < d₂₀, d_(2m)(nm) = 68.38 126.05 181.56 22.38 72.33 Case 2-11 2-12 2-13 2-14 2-15 n₁₀ 1.7364 1.7194 1.7189 1.7279 1.7039 k₁₀ 0.0767 0.0663 0.0609 0.0714 0.0620 d₁₀(nm) 160.57 160.35 240.33 230.11 268.01 n₂₀ 1.7865 1.6960 2.2401 1.8887 1.7359 k₂₀ 0.2463 0.1988 0.7138 0.3299 0.2398 d₂₀(nm) 145.39 214.32 17.92 78.86 158.55 for n₁ ≧ n₁₀, n_(1m) = 1.7918 1.7729 1.7932 1.7879 1.7579 for n₁ < n₁₀, n_(1m) = 1.7262 1.6947 1.6903 1.7176 1.6407 for k₁ ≧ k₁₀, k_(1m) = 0.1172 0.1176 0.1266 0.1177 0.1322 for k₁ < k₁₀, k_(1m) = 0.0534 0.0312 0.0317 0.0558 0.0228 for d₁ ≧ d₁₀, d_(1m)(nm) = 198.97 ∞ ∞ ∞ ∞ for d₁ < d₁₀, d_(1m)(nm) = 157.73 149.13 225.89 226.73 223.91 for n₂ ≧ n₂₀, n_(2m) = 1.8969 1.9046 2.4255 2.0020 1.9149 for n₂ < n₂₀, n_(2m) = 1.6706 1.5895 2.0733 1.8277 1.4543 for k₂ ≧ k₂₀, k_(2m) = 0.3435 0.2910 0.8416 0.3876 0.4261 for k₂ < k₂₀, k_(2m) = 0.1729 0.1351 0.5371 0.2258 0.1424 for d₂ ≧ d₂₀, d_(2m)(nm) = 161.62 ∞ 21.50 87.70 ∞ for d₂ < d₂₀, d_(2m)(nm) = 139.39 187.96 15.15 76.00 129.53 Case 2-16 n₁₀ 1.7046 k₁₀ 0.0595 d₁₀(nm) 264.54 n₂₀ 1.7170 k₂₀ 0.1955 d₂₀(nm) 223.28 for n₁ ≧ n₁₀, n_(1m) = 1.7716 for n₁ < n₁₀, n_(1m) = 1.6465 for k₁ ≧ k₁₀, k_(1m) = 0.1321 for k₁ < k₁₀, k_(1m) = 0.0178 for d₁ ≧ d₁₀, d_(1m)(nm) = ∞ for d₁ < d₁₀, d_(1m)(nm) = 160.48 for n₂ ≧ n₂₀, n_(2m) = 2.1001 for n₂ < n₂₀, n_(2m) = 1.4760 for k₂ ≧ k₂₀, k_(2m) = 0.4081 for k₂ < k₂₀, k_(2m) = 0.1085 for d₂ ≧ d₂₀, d_(2m)(nm) = ∞ for d₂ < d₂₀, d_(2m)(nm) = 143.86

According to a third embodiment of the present invention, there is provided an antireflection film having a two-layer structure and formed between a resist layer and a surface of a silicon semiconductor substrate for being used when the resist layer is exposed by an exposure system which is used in a fabrication process of a semiconductor device and has a wavelength of 190 nm to 195 nm and a numerical aperture more than 1.1 but equal to or less than 1.2. Further, according to the third embodiment of the present invention, there is provided an exposure method for exposing a resist layer by means of an exposure system which is used in a fabrication process of a semiconductor device and has a wavelength of 190 nm to 195 nm and a numerical aperture more than 1.1 but equal to or less than 1.2, an antireflection film which has a two-layer structure being formed between the resist layer and a surface of a silicon semiconductor substrate.

The antireflection film and the exposure method according to the third embodiment are configured such that the-antireflection film includes an upper layer having a complex refractive index N₁ equal to n₁−k₁i and a film thickness d₁ whose unit is nm, and a lower layer having a complex refractive index N₂ equal to n₂−k₂i and a film thickness d₂ whose unit is nm, the upper layer and the lower layer being configured such that, when one of cases [3-01] to [3-14] defined in a table given below is selected as a combination of values of [n₁₀, k₁₀, d₁₀, n₂₀, k₂₀, d₂₀], n₁, k₁, d₁, n₂, k₂ and d₂ satisfy an expression {(n ₁-n ₁₀)/(n _(1m)-n ₁₀)}²+{(k ₁-k ₁₀)/(k _(1m)-k ₁₀)}²+{(d ₁-d ₁₀)/(d _(1m)-d ₁₀)}²+{(n ₂-n ₂₀)/(n _(2m)-n ₂₀)}²+{(k ₂-k ₂₀) /(k _(2m)-k ₂₀)}²+{(d ₂-d ₂₀)/(d_(2m)-d ₂₀)}²≦1 where a value of n_(1m) in the pertaining case is adopted between on a relationship in magnitude between n₁ and n₁₀, a value of k_(1m) in the pertaining case is adopted between on a relationship in magnitude between k₁ and k₁₀, a value of d_(1m) in the pertaining case is adopted between on a relationship in magnitude between d₁ and d₁₀, a value of n_(2m) in the pertaining case is adopted between on a relationship in magnitude between n₂ and n₂₀, a value of k_(2m) in the pertaining case is adopted between on a relationship in magnitude between k₂ and k₂₀, and a value of d_(2m) in the pertaining case is adopted between on a relationship in magnitude between d₂ and d₂₀.

Case 3-01 3-02 3-03 3-04 3-05 n₁₀ 2.1010 1.9972 1.8971 1.8903 1.7614 k₁₀ 0.0000 0.1417 0.0932 0.1047 0.0933 d₁₀(nm) 18.86 29.97 20.09 13.40 99.78 n₂₀ 2.3980 3.9849 1.8912 1.7190 1.8773 k₂₀ 0.9577 0.5156 0.3589 0.2691 0.6361 d₂₀(nm) 20.51 29.99 144.86 225.69 29.70 for n₁ ≧ n₁₀, n_(1m) = 2.1902 2.0806 1.9757 1.9938 1.8213 for n₁ < n₁₀, n_(1m) = 2.0333 1.9400 1.8442 1.8243 1.7445 for k₁ ≧ k₁₀, k_(1m) = 0.0791 0.2081 0.1538 0.1917 0.1313 for k₁ < k₁₀, k_(1m) = 0.0000 0.0680 0.0073 0.0023 0.0538 for d₁ ≧ d₁₀, d_(1m)(nm) = 22.17 34.24 27.46 20.29 118.37 for d₁ < d₁₀, d_(1m)(nm) = 16.20 26.95 16.03 9.40 96.05 for n₂ ≧ n₂₀, n_(2m) = 2.5150 4.1060 2.0062 1.8367 1.9517 for n₂ < n₂₀, n_(2m) = 2.2758 3.8579 1.7470 1.5737 1.7548 for k₂ ≧ k₂₀, k_(2m) = 1.0902 0.6644 0.5181 0.3688 0.7101 for k₂ < k₂₀, k_(2m) = 0.8269 0.4039 0.2637 0.1833 0.5274 for d₂ ≧ d₂₀, d_(2m)(nm) = 23.39 31.19 ∞ ∞ 33.13 for d₂ < d₂₀, d_(2m)(nm) = 17.92 28.87 85.53 141.88 25.36 Case 3-06 3-07 3-08 3-09 3-10 n₁₀ 1.7825 1.7569 1.7277 1.7272 1.7147 k₁₀ 0.0898 0.0868 0.0740 0.0744 0.0633 d₁₀(nm) 97.07 96.31 94.69 178.89 164.15 n₂₀ 2.0041 1.7847 1.6779 2.1865 1.6838 k₂₀ 0.3750 0.2610 0.2014 0.6947 0.1862 d₂₀(nm) 75.78 148.77 220.98 19.20 215.48 for n₁ ≧ n₁₀, n_(1m) = 1.8327 1.7995 1.7711 1.7845 1.7573 for n₁ < n₁₀, n_(1m) = 1.7698 1.7544 1.7097 1.7167 1.6822 for k₁ ≧ k₁₀, k_(1m) = 0.1223 0.0982 0.1152 0.1077 0.1011 for k₁ < k₁₀, k_(1m) = 0.0533 0.0642 0.0321 0.0488 0.0264 for d₁ ≧ d₁₀, d_(1m)(nm) = 109.28 111.91 114.36 218.45 ∞ for d₁ < d₁₀, d_(1m)(nm) = 94.62 95.76 89.11 175.03 147.22 for n₂ ≧ n₂₀, n_(2m) = 2.0899 1.8293 1.7201 2.2837 1.7321 for n₂ < n₂₀, n_(2m) = 1.9035 1.6980 1.5934 2.0604 1.6046 for k₂ ≧ k₂₀, k_(2m) = 0.4366 0.3015 0.2464 0.7527 0.2137 for k₂ < k₂₀, k_(2m) = 0.2899 0.2021 0.1479 0.5549 0.1380 for d₂ ≧ d₂₀, d_(2m)(nm) = 81.59 161.61 ∞ 21.11 235.37 for d₂ < d₂₀, d_(2m)(nm) = 70.00 146.51 196.47 16.79 195.03 Case 3-11 3-12 3-13 3-14 n₁₀ 1.7036 1.7000 1.7012 1.7028 k₁₀ 0.0666 0.0723 0.0708 0.0661 d₁₀(nm) 228.90 216.03 209.55 205.70 n₂₀ 2.1518 1.7881 1.7244 1.7099 k₂₀ 0.6409 0.3189 0.2345 0.1906 d₂₀(nm) 21.01 93.79 164.15 230.44 for n₁ ≧ n₁₀, n_(1m) = 1.7333 1.7203 1.7336 1.7514 for n₁ < n₁₀, n_(1m) = 1.6243 1.6387 1.6472 1.6539 for k₁ ≧ k₁₀, k_(1m) = 0.1086 0.1103 0.1181 0.1191 for k₁ < k₁₀, k_(1m) = 0.0356 0.0460 0.0368 0.0268 for d₁ ≧ d₁₀, d_(1m)(nm) = ∞ 227.26 237.88 ∞ for d₁ < d₁₀, d_(1m)(nm) = 181.97 190.09 179.63 173.04 for n₂ ≧ n₂₀, n_(2m) = 2.3031 1.9012 1.8497 1.8964 for n₂ < n₂₀, n_(2m) = 2.0795 1.7532 1.6568 1.5385 for k₂ ≧ k₂₀, k_(2m) = 0.7063 0.3281 0.3333 0.3179 for k₂ < k₂₀, k_(2m) = 0.5137 0.2264 0.1529 0.1170 for d₂ ≧ d₂₀, d_(2m)(nm) = 24.52 111.38 ∞ ∞ for d₂ < d₂₀, d_(2m)(nm) = 19.07 89.55 150.63 157.43

According to a fourth embodiment of the present invention, there is provided an antireflection film having a two-layer structure and formed between a resist layer and a surface of a silicon semiconductor substrate for being used when the resist layer is exposed by an exposure system which is used in a fabrication process of a semiconductor device and has a wavelength of 190 nm to 195 nm and a numerical aperture more than 1.2 but equal to or less than 1.3. Further, according to the fourth embodiment of the present invention, there is provided an exposure method for exposing a resist layer by means of an exposure system which is used in a fabrication process of a semiconductor device and has a wavelength of 190 nm to 195 nm and a numerical aperture more than 1.2 but equal to or less than 1.3, an antireflection film which has a two-layer structure being formed between the resist layer and a surface of a silicon semiconductor substrate.

The antireflection film and the exposure method according to the fourth embodiment are configured such that the antireflection film includes an upper layer having a complex refractive index N₁ equal to n₁−k₁i and a film thickness d₁ whose unit is nm, and a lower layer having a complex refractive index N₂ equal to n₂−k₂i and a film thickness d₂ whose unit is nm, the upper layer and the lower layer being configured such that, when one of cases [4-01] to [4-10] defined in a table given below is selected as a combination of values of [n₁₀, k₁₀, d₁₀, n₂₀, k₂₀, d₂₀], n₁, k₁, d₁, n₂, k₂ and d₂ satisfy an expression {(n ₁-n ₁₀)/(n _(1m)-n ₁₀)}²+{(k ₁-k ₁₀)/(k _(1m)-k ₁₀)}²+{(d ₁-d ₁₀)/(d _(1m)-d ₁₀)}²+{(n ₂-n ₂₀)/(n _(2m)-n ₂₀)}²+{(k ₂-k ₂₀) /(k _(2m)-k ₂₀)}²+{(d ₂-d ₂₀)/(d _(2m)-d ₂₀)}²≦1 where a value of n_(1m) in the pertaining case is adopted between on a relationship in magnitude between n₁ and n₁₀, a value of k_(1m) in the pertaining case is adopted between on a relationship in magnitude between k₁ and k₁₀, a value of d_(1m) in the pertaining case is adopted between on a relationship in magnitude between d₁ and d₁₀, a value of n_(2m) in the pertaining case is adopted between on a relationship in magnitude between n₂ and n₂₀, a value of k_(2m) in the pertaining case is adopted between on a relationship in magnitude between k₂ and k₂₀, and a value of d_(2m) in the pertaining case is adopted between on a relationship in magnitude between d₂ and d₂₀.

Case 4-01 4-02 4-03 4-04 4-05 n₁₀ 2.0750 2.0118 1.8885 1.8806 1.7567 k₁₀ 0.0000 0.1190 0.0999 0.1003 0.0923 d₁₀(nm) 20.30 29.87 17.71 13.44 108.92 n₂₀ 2.4310 4.0092 1.7811 1.7062 2.0485 k₂₀ 0.9366 0.5022 0.3211 0.2477 0.6631 d₂₀(nm) 19.90 29.99 159.56 227.84 23.68 for n₁ ≧ n₁₀, n_(1m) = 2.1541 2.0844 1.9589 1.9713 1.7997 for n₁ < n₁₀, n_(1m) = 2.0215 1.9638 1.8538 1.8291 1.7557 for k₁ ≧ k₁₀, k_(1m) = 0.0610 0.1705 0.1459 0.1729 0.0954 for k₁ < k₁₀, k_(1m) = 0.0000 0.0518 0.0187 0.0078 0.0655 for d₁ ≧ d₁₀, d_(1m)(nm) = 23.54 33.58 23.82 19.76 125.01 for d₁ < d₁₀, d_(1m)(nm) = 18.03 27.42 15.13 10.09 108.67 for n₂ ≧ n₂₀, n_(2m) = 2.5291 4.1084 1.8635 1.7809 2.0547 for n₂ < n₂₀, n_(2m) = 2.3203 3.9019 1.6624 1.5899 1.9572 for k₂ ≧ k₂₀, k_(2m) = 1.0610 0.6325 0.4092 0.3139 0.6691 for k₂ < k₂₀, k_(2m) = 0.8178 0.4040 0.2433 0.1776 0.5710 for d₂ ≧ d₂₀, d_(2m)(nm) = 22.43 30.97 ∞ ∞ 23.86 for d₂ < d₂₀, d_(2m)(nm) = 17.62 29.03 129.86 149.42 21.22 Case 4-06 4-07 4-08 4-09 4-10 n₁₀ 1.7300 1.7016 1.7036 1.7088 1.7083 k₁₀ 0.0690 0.0665 0.0722 0.0700 0.0641 d₁₀(nm) 99.33 227.28 216.05 208.98 205.66 n₂₀ 1.7059 2.1201 1.7959 1.7311 1.7076 k₂₀ 0.1911 0.6392 0.3181 0.2343 0.1900 d₂₀(nm) 215.34 21.82 93.13 163.14 228.20 for n₁ ≧ n₁₀, n_(1m) = 1.7599 1.7325 1.7213 1.7343 1.7487 for n₁ < n₁₀, n_(1m) = 1.7290 1.6697 1.6816 1.6905 1.6839 for k₁ ≧ k₁₀, k_(1m) = 0.0744 0.1071 0.1083 0.1002 0.0965 for k₁ < k₁₀, k_(1m) = 0.0522 0.0350 0.0475 0.0408 0.0326 for d₁ ≧ d₁₀, d_(1m)(nm) = 114.51 249.66 226.44 234.14 ∞ for d₁ < d₁₀, d_(1m)(nm) = 98.99 206.91 203.38 198.02 187.04 for n₂ ≧ n₂₀, n_(2m) = 1.7114 2.2630 1.9107 1.8583 1.8700 for n₂ < n₂₀, n_(2m) = 1.6501 2.0448 1.7644 1.6757 1.5497 for k₂ ≧ k₂₀, k_(2m) = 0.1929 0.7020 0.3809 0.3287 0.3066 for k₂ < k₂₀, k_(2m) = 0.1524 0.5119 0.2256 0.1573 0.1188 for d₂ ≧ d₂₀, d_(2m)(nm) = 219.55 25.26 110.64 ∞ ∞ for d₂ < d₂₀, d_(2m)(nm) = 205.88 19.68 89.45 150.12 160.78

According to a fifth embodiment of the present invention, there is provided an antireflection film having a two-layer structure and formed between a resist layer and a surface of a silicon semiconductor substrate for being used when the resist layer is exposed by an exposure system which is used in a fabrication process of a semiconductor device and has a wavelength of 190 nm to 195 nm and a numerical aperture more than 1.3 but equal to or less than 1.4. Further, according to the first embodiment of the present invention, there is provided an exposure method for exposing a resist layer by means of an exposure system which is used in a fabrication process of a semiconductor device and has a wavelength of 190 nm to 195 nm and a numerical aperture more than 1.3 but equal to or less than 1.4, an antireflection film which has a two-layer structure being formed between the resist layer and a surface of a silicon semiconductor substrate.

The antireflection film and the exposure method according to the fifth embodiment are configured such that the antireflection film includes an upper layer having a complex refractive index N₁ equal to n₁−k₁i and a film thickness d₁ whose unit is nm, and a lower layer having a complex refractive index N₂ equal to n₂−k₂i and a film thickness d₂ whose unit is nm, the upper layer and the lower layer being configured such that, when one of cases [5-01] to [5-07] defined in a table given below is selected as a combination of values of [n₁₀, k₁₀, d₁₀, n₂₀, k₂₀, d₂₀], n₁, k₁, d₁, n₂, k2 and d₂ satisfy an expression {(n ₁-n ₁₀)/(n _(1m)-n ₁₀)}²+{(k ₁-k ₁₀)/(k _(1m)-k ₁₀)}²+{(d ₁-d ₁₀)/(d _(1m)-d ₁₀)}²+{(n ₂-n ₂₀)/(n _(2m)-n ₂₀)}²+{(k ₂-k ₂₀) /(k _(2m)-k ₂₀)}²+{(d ₂-d ₂₀)/(d _(2m)-d ₂₀)}²≦1 where a value of n_(1m) in the pertaining case is adopted between on a relationship in magnitude between n₁ and n₁₀, a value of k_(1m) in the pertaining case is adopted between on a relationship in magnitude between k₁ and k₁₀, a value of d_(1m) in the pertaining case is adopted between on a relationship in magnitude between d₁ and d₁₀, a value of n_(2m) in the pertaining case is adopted between on a relationship in magnitude between n₂ and n₂₀, a value of k_(2m) in the pertaining case is adopted between on a relationship in magnitude between k₂ and k₂₀, and a value of d_(2m) in the pertaining-case is adopted between on a relationship in magnitude between d₂ and d₂₀.

Case 5-01 5-02 5-03 5-04 5-05 n₁₀ 2.0901 2.0375 1.8787 1.8780 1.7009 k₁₀ 0.0000 0.0819 0.1028 0.0706 0.0609 d₁₀(nm) 20.79 29.12 16.60 14.89 160.18 n₂₀ 2.4315 3.6552 1.7172 1.7467 1.6995 k₂₀ 0.9254 0.4960 0.2840 0.2361 0.1745 d₂₀(nm) 20.34 34.09 167.85 221.06 215.71 for n₁ ≧ n₁₀, n_(1m) = 2.1532 2.0916 1.9323 1.9461 1.7131 for n₁ < n₁₀, n_(1m) = 2.0485 1.9946 1.8625 1.8482 1.6965 for k₁ ≧ k₁₀, k_(1m) = 0.0301 0.1157 0.1287 0.1125 0.0797 for k₁ < k₁₀, k_(1m) = 0.0000 0.0234 0.0358 0.0000 0.0529 for d₁ ≧ d₁₀, d_(1m)(nm) = 23.53 31.97 21.01 20.40 168.49 for d₁ < d₁₀, d_(1m)(nm) = 19.45 27.24 15.35 12.65 156.71 for n₂ ≧ n₂₀, n_(2m) = 2.4915 3.7301 1.7470 1.7894 1.7056 for n₂ < n₂₀, n_(2m) = 2.3369 3.5977 1.6335 1.6492 1.6786 for k₂ ≧ k₂₀, k_(2m) = 1.0253 0.5706 0.3145 0.2771 0.1981 for k₂ < k₂₀, k_(2m) = 0.8408 0.4125 0.2297 0.1801 0.1502 for d₂ ≧ d₂₀, d_(2m)(nm) = 22.48 35.05 ∞ ∞ 219.96 for d₂ < d₂₀, d_(2m)(nm) = 18.31 33.41 144.47 152.04 200.15 Case 5-06 5-07 n₁₀ 1.7204 1.7142 k₁₀ 0.0677 0.0552 d₁₀(nm) 231.66 225.66 n₂₀ 2.2460 1.7026 k₂₀ 0.6523 0.1831 d₂₀(nm) 18.88 210.32 for n₁ ≧ n₁₀, n_(1m) = 1.7346 1.7449 for n₁ < n₁₀, n_(1m) = 1.7142 1.7015 for k₁ ≧ k₁₀, k_(1m) = 0.0791 0.0776 for k₁ < k₁₀, k_(1m) = 0.0480 0.0279 for d₁ ≧ d₁₀, d_(1m)(nm) = 241.66 269.84 for d₁ < d₁₀, d_(1m)(nm) = 227.75 215.83 for n₂ ≧ n₂₀, n_(2m) = 2.3315 1.8141 for n₂ < n₂₀, n_(2m) = 2.2068 1.6257 for k₂ ≧ k₂₀, k_(2m) = 0.6941 0.2591 for k₂ < k₂₀, k_(2m) = 0.5188 0.1258 for d₂ ≧ d₂₀, d_(2m)(nm) = 20.91 ∞ for d₂ < d₂₀, d_(2m)(nm) = 17.96 186.01

The exposure methods according to the first to fifth embodiments of the present invention are applied, for example, to working of a very fine pattern of a semiconductor device and particularly include a step of forming an antifriction film of the present invention on a silicon semiconductor substrate, a step of applying and forming a resist layer having a photosensitive action to and on the antireflection layer, a step of selectively exposing the resist layer with exposure light (ultraviolet rays), and a step of developing the resist layer to obtain a predetermined resist pattern.

In the antireflection films according to the first to fifth embodiments of the present invention or the exposure methods according to the first to fifth embodiments of the present invention (in the following description, the antireflection films and the exposure methods are sometimes referred to collectively as present invention), the exposure light (illumination light) has a wavelength of 190 nm to 195 nm. However, the exposure light (illumination light) preferably has a wavelength of 192 nm to 194 nm, and more preferably, an ArF excimer laser of a wavelength of 193 nm is used as the exposure light source.

Further, it is preferable to satisfy d₁≦250 and besides satisfy d₂≦250. In other words, preferably the film thickness of the upper layer of the antireflection film does not exceed 250 nm and besides also the film thickness of the lower layer does not exceed 250 nm. If the film thickness of the upper layer exceeds 250 nm or the film thickness of the lower layer exceeds 250 nm, then at a step of etching a silicon semiconductor substrate using a resist layer as an etching mask after the resist layer is exposed with exposure light and developed, the work conversion difference (also called dimension conversion amount or dimension shift) which is a difference between a resist pattern dimension of the resist layer and an etching work dimension of an actual silicon semiconductor substrate may become excessively great, resulting in the possibility that a pattern having a desired shape or size may not be obtained on the silicon semiconductor substrate.

Further, the refractive index of the resist layer preferably ranges from 1.60 to 1.80. Where a resist film made of a resist material whose refractive index does not fall within the range, even if the antireflection film satisfies any of the sets of conditions of (n₁, k₁, d₁, n₂, k₂, d₂) described hereinabove, it may be difficult to suppress the reflectance at the interface between the resist layer and the silicon semiconductor substrate to 0.4% or less over the overall region from an incident angle (maximum incident angle θ_(in-max)) of exposure light corresponding to the pertaining numerical aperture to the perpendicular incidence (minimum incident angle θ_(in-min)), resulting in the possibility that a good resist pattern shape may not be obtained.

It is to be noted that, in the following description, the overall region from the incident angle (maximum incident angle θ_(in-max)) of the exposure light corresponding to the pertaining numerical aperture to the perpendicular incidence (minimum incident angle θ_(in-min)) is sometimes referred to as “overall region of the incident angle corresponding to the pertaining numerical aperture NA of the exposure system” or merely as “overall region of the incident angle”.

Further, preferably the film thickness of the resist layer is equal to approximately 2 to 5 times that of the minimum resist pattern size to be formed. Although the film thickness of the resist layer is smaller than twice the minimum resist pattern size, it is possible to pattern the resist layer so as to have a predetermined pattern. However, when the silicon semiconductor substrate is etched after the patterning of the resist layer, there is the possibility that a good etching result may not be obtained. In addition, there is the possibility also that the number of film defects in the resist layer may increase. On the other hand, where the film thickness of the resist layer exceeds five times the minimum resist pattern size, there is the possibility that the pattern resist layer may collapse and a good patterning result of the silicon semiconductor substrate may not be obtained.

The material which forms each of the upper and lower layers of the antireflection film may be any material only if it satisfies any of the various sets of conditions of (n₁, k₁, d₁, n₂, k₂, d₂) described hereinabove. For example, as the materials for forming the upper and lower layers, polymer materials, inorganic oxide materials, metal materials and hybrid materials of them may be used. In particular, for example, polyimide films, SiCH films, SiCHN films, epoxy type thermal-cure resin films, acrylic type thermal-cure resin films, epoxy type ultraviolet curing resin films and acrylic type ultraviolet curing resin films may be used.

It is to be noted that, for the object of protection and so forth of the resist layer, a protective layer made of an organic substance or an inorganic substance, particularly a protective film made of, for example, polyvinyl alcohol, amorphous fluoropolymer or NaCl, may be provided on the resist film.

Further, in order to enhance the close contact and so forth between the resist layer formed on the antireflection film and the antireflection film, a surface reforming process by a silane coupling agent or the like may be performed for the surface of the upper layer which forms the antireflection film.

Usually, in a single-layer antireflection film, in whatever manner the film thickness and the complex refraction index are varied, it is impossible to suppress the reflectance to 0.4% or less over the overall region of the incident angle corresponding to the pertaining numerical aperture NA of the exposure system. Further, if the film thickness of the antireflection film is excessively great, then the problem of the work conversion difference occurs at a step of etching the silicon semiconductor substrate after the resist layer is exposed with exposure light and developed.

On the other hand, in the present invention, since the antireflection film of a two-layer configuration having a film thickness and a complex refraction factor which are individually within predetermined ranges is formed between the resist layer and the silicon semiconductor substrate, it is possible to suppress the reflectance to 0.4% or less over the overall region of the incoming angle corresponding to the pertaining numerical aperture NA of the exposure system. Consequently, a resist pattern having a better shape can be obtained, and very fine working much finer than ever can be anticipated. In other words, where the film thickness and the complex refractive index of the antireflection film of a two-layer configuration satisfy the conditions described hereinabove in the case wherein the numerical aperture of the exposure system is within the ranges of NA≦1.0, 1.0<NA≦1.1, 1.1<NA≦1.2, 1.2<NA≦1.3 and 1.3<NA≦1.4, the reflectance can be set to 0.4% or less over the overall region from the incident angle of the exposure light corresponding to the pertaining numerical aperture NA to the perpendicular incidence. As a result, a resist pattern of a good shape can be obtained. Further, the work conversion difference can be suppressed low.

The above and other objects, features and advantages of the present invention will become apparent from the following description and the appended claims, taken in conjunction with the accompanying drawings in which like parts or elements denoted by like reference symbols.

BRIEF DESCRIPTION OF THE DRAWINGS

FIG. 1 is a table illustrating maximum values, determined by theoretical calculation, of the reflectance in a condition wherein the reflectance of the perpendicular incidence side is minimized from an incident angle where exposure light enters most obliquely corresponding to the numerical aperture of an exposure system with regard to various film thicknesses of an upper layer and a lower which form an antireflection film where the numerical aperture of the exposure system is 1.0;

FIG. 2 is a table illustrating maximum values, determined by theoretical calculation, of the reflectance in a condition wherein the reflectance of the perpendicular incidence side is minimized from an incident angle where exposure light enters most obliquely corresponding to the numerical aperture of an exposure system with regard to various film thicknesses of an upper layer and a lower which form an antireflection film where the numerical aperture of the exposure system is 1.1;

FIG. 3 is a table illustrating maximum values, determined by theoretical calculation, of the reflectance in a condition wherein the reflectance of the perpendicular incidence side is minimized from an incident angle where exposure light enters most obliquely corresponding to the numerical aperture of an exposure system with regard to various film thicknesses of an upper layer and a lower which form an antireflection film where the numerical aperture of the exposure system is 1.2;

FIG. 4 is a table illustrating maximum values, determined by theoretical calculation, of the reflectance in a condition wherein the reflectance of the perpendicular incidence side is minimized from an incident angle where exposure light enters most obliquely corresponding to the numerical aperture of an exposure system with regard to various film thicknesses of an upper layer and a lower which form an antireflection film where the numerical aperture of the exposure system is 1.3; and

FIG. 5 is a table illustrating maximum values, determined by theoretical calculation, of the reflectance in a condition wherein the reflectance of the perpendicular incidence side is minimized from an incident angle where exposure light enters most obliquely corresponding to the numerical aperture of an exposure system with regard to various film thicknesses of an upper layer and a lower which form an antireflection film where the numerical aperture of the exposure system is 1.4.

DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

Before preferred embodiments of the present invention are described with reference to the accompanying drawings, the reason why, where the present invention is applied, the reflectance is suppressed to 0.4% or less over an overall region of the incident angle corresponding to the pertaining numerical aperture NA of an exposure system (overall region from the incident angle of the exposure light corresponding to the numerical aperture NA of the exposure system to the perpendicular incidence) is described.

An optimization simulation of complex refractive indices N₁ and N₂ of an upper layer and a lower layer of an antireflection film was conducted such that the reflectance where the numerical aperture NA of the exposure system was set to 1.0, 1.1, 1.2, 1.3 and 1.4 from an incident angle (maximum incident angle θ_(in-max)) from the corresponding most oblique direction to the perpendicular incidence (minimum incident angle θ_(in-min)=0 degree), that is, over the overall region of the incident angle, was minimized in individual combinations of values at increments of 10 nm of the film thickness d₁ of the upper layer from 10 nm to 250 nm and values at increments of 10 nm of the film thickness d₂ of the lower layer from 10 nm to 250 nm.

In the calculation described above, for the calculation of the reflectance of the two-layer antireflection film, a calculation method based on a character matrix (refer to Mitsunobu KOBIYAMA, Basic Theories of an Optical Thin Film, Optronics, 2003) was adopted. For the optimization of the complex refractive indices of the upper layer and the lower layer, the optimization method of Fletcher-Reeves (refer to J. Kowalik and M. R. Osborne, Methods for Unconstrained Optimization Probrems, translated by Yoshiyuki YAMAMOTO and Takeo KOYAMA, Baifukan, 1970) was applied.

Upon optimization, where the numerical aperture NA was 1.0, the overall region of the incident angle is divided into twenty equal parts. Then, the reflectance at each incident angle was calculated, and the square sum of the reflectances at the incident angles was minimized. It is to be noted that, for the values 1.1, 1.2, 1.3 and 1.4 of the numerical aperture NA, similar calculation was performed using values of the reflectance at incident angles where the overall region of the incident angle was divided into 22 equal parts, 24 equal parts, 26 equal parts and 28 equal parts, respectively.

By performing optimization of the complex refractive indices of the upper layer and the lower layer of the antireflection film using the method described above for each of combinations wherein the numerical aperture NA of the exposure system is successively changed to 1.0, 1.1, 1.2, 1.3 and 1.4 and the film thickness d₁ of the upper layer is successively changed to increments of 10 nm from 10 nm to 250 nm while the film thickness d₂ of the lower layer is successively changed to increments of 10 nm from 10 nm to 250 nm in such a manner as described above, optimum complex refractive indices N₁ and N₂ for the upper layer and the lower layer were obtained. Using the complex refractive indices N₁ and N₂ of the upper layer and the lower obtained in this manner, maximum values among reflectances within a range from the most oblique incident angle (maximum incident angle θ_(in-max)) corresponding to the numerical aperture NA of the pertaining exposure system to the vertical incident angle (minimum incident angle θ_(in-min)), that is, within the overall range of the incident angle, were determined. Results of the determination are illustrated in FIGS. 1 to 5. It is to be noted that FIGS. 1 to 5 illustrate maximum values, determined from theoretical calculation, of the reflectance in the condition that the reflectance is minimized over the overall region of the incident angle (optimum complex refractive indices N₁ and N₂ of the upper layer and the lower layer) at the film thicknesses d₁ and d₂ of the upper layer and the lower layer where the numerical aperture NA of the exposure system is 1.0, 1.1, 1.2, 1.3 and 1.4, respectively.

As recognized from FIGS. 1 to 5, a film thickness condition that the maximum reflectance is equal to or less than 0.4% exists at each of the values of the numerical aperture NA.

It is to be noted that the reason why calculation for a case wherein the film thickness is greater than 250 nm was not performed is that, where the film thickness is greater than 250 nm, the work conversion difference at an etching step becomes so great that good working of a silicon semiconductor substrate cannot be anticipated.

The condition that the maximum reflectance is within a region equal to or lower than 0.4% in each of FIGS. 1 to 5 from among the film thickness conditions in which the square sum of the reflectances which is an evaluation function for optimization is minimized in each of the cases wherein the numerical aperture NA of the exposure system is set to 1.0, 1.1, 1.2, 1.3 and 1.4 and the film thickness d₁ of the upper layer is varied by an increment of 10 nm from 10 nm to 250 nm while the film thickness d₂ of the lower layer is varied by an increment from 10 nm to 250 nm is the most preferable film thickness condition. Further, corresponding complex refraction indexes of the upper and lower layers of the film thickness condition are the most preferable complex refractive indices.

Then, based on FIGS. 1 to 5, the film thickness d₁ of the upper layer and the film thickness d₂ of the lower layer were further optimized.

As a result, the most preferable combinations of the complex refractive indices and the film thickness given below were obtained. In particular, where the complex refractive index of the upper layer (layer positioned remotely from the surface of the silicon semiconductor substrate) of the two-layer antireflection film is represented by N₁ while the complex refractive index of the lower layer (layer formed on the surface of the silicon semiconductor substrate) is represented by N₂ and the complex refractive indices N₁ and N₂ are defined by N ₁ =n ₁₀ −k ₁₀ i N ₂ =n ₂₀ −k ₂₀ i and besides the film thickness (unit: nm) of the upper layer is represented by d₁₀ and the film thickness (unit: nm) of the lower layer is represented by d₂₀, combinations of values of [n₁₀, n₂₀, k₁₀, k₂₀, d₁₀, d₂₀] illustrated in Table 1 and Table 2 given below are the most preferable combinations, that is, combinations with which a minimum value of-the reflectance is obtained. It is to be that [case A-01] to [case A-16] are values for NA=1.0; [case B-01] to [case B-16] are values for NA=1.1; [case C-01] to [case C-14] are values for NA=1.2; [case D-01] to [case D-10] are values for NA=1.3; and [case E-01] to [case E-07] are values for NA=1.4. In the conditions described above, for NA=1.0, a minimum value of the reflectance is obtained at 16 points (16 combinations of [n₁₀, n₂₀, k₁₀, k₂₀, d₁₀, d₂₀]); for NA=1.1, a minimum value of the reflectance is obtained at 16 points (16 combinations of [n₁₀, n₂₀, k₁₀, k₂₀, d₁₀, d₂₀]) ; for NA=1.2, a minimum value of the reflectance is obtained at 14 points (14 combinations of [n₁₀, n₂₀, k₁₀, k₂₀, d₁₀, d₂₀]); for NA=1.3, a minimum value of the reflectance is obtained at 10 points (10 combinations of [n₁₀, n₂₀, k₁₀, k₂₀, d₁₀, d₂₀]); and for NA=1.4, a minimum value of the reflectance is obtained at 7 points (7 combinations of [n₁₀, n₂₀, k₁₀, k₂₀, d₁₀, d₂₀])

TABLE 1 Case A-01 A-02 A-03 A-04 A-05 A-06 A-07 A-08 n₁₀ 2.1616 1.9575 1.8783 1.8886 1.7671 1.7783 1.7756 1.7637 k₁₀ 0.0031 0.1578 0.1120 0.0828 0.0972 0.0854 0.0827 0.0788 d₁₀(nm) 16.39 29.70 22.79 17.43 89.65 90.09 89.16 88.60 n₂₀ 2.3326 3.1421 1.9535 1.8540 1.7266 1.9451 1.8813 1.8074 k₂₀ 0.9955 0.5540 0.3987 0.3157 0.6265 0.4110 0.2980 0.2358 d₂₀(nm) 21.81 39.99 133.42 201.01 35.79 78.70 136.86 201.53 Case A-09 A-10 A-11 A-12 A-13 A-14 A-15 A-16 n₁₀ 1.7297 1.7402 1.7416 1.7346 1.7204 1.7293 1.7290 1.7210 k₁₀ 0.0695 0.0705 0.0723 0.0700 0.0573 0.0638 0.0672 0.0630 d₁₀(nm) 159.09 157.00 154.81 154.48 226.55 221.51 219.00 220.18 n₂₀ 1.8027 1.9115 1.8276 1.7635 1.9505 1.9167 1.7992 1.7329 k₂₀ 0.6176 0.3647 0.2602 0.2082 0.6496 0.3426 0.2416 0.1973 d₂₀(nm) 30.94 79.38 140.99 205.63 25.08 78.00 142.68 207.16 Case B-01 B-02 B-03 B-04 B-05 B-06 B-07 B-08 n₁₀ 2.1270 1.9689 1.8874 1.9059 1.7643 1.7803 1.7743 1.7445 k₁₀ 0.0000 0.1461 0.1027 0.0744 0.0947 0.0868 0.0850 0.0789 d₁₀(nm) 17.47 29.67 21.38 15.49 94.08 93.23 91.77 92.02 n₂₀ 2.3628 3.1616 1.9199 1.8297 1.7955 1.9791 1.8636 1.7368 k₂₀ 0.9776 0.5440 0.3802 0.2998 0.6320 0.3951 0.2810 0.2206 d₂₀(nm) 21.04 39.98 139.31 207.65 32.98 77.05 139.87 212.33 Case B-09 B-10 B-11 B-12 B-13 B-14 B-15 B-16 n₁₀ 1.7294 1.7425 1.7364 1.7194 1.7189 1.7279 1.7039 1.7046 k₁₀ 0.0717 0.0762 0.0767 0.0663 0.0609 0.0714 0.0620 0.0595 d₁₀(nm) 166.39 161.95 160.57 160.35 240.33 230.11 268.01 264.54 n₂₀ 1.9163 1.9299 1.7865 1.6960 2.2401 1.8887 1.7359 1.7170 k₂₀ 0.6369 0.3467 0.2463 0.1988 0.7138 0.3299 0.2398 0.1955 d₂₀(nm) 26.72 78.23 145.39 214.32 17.92 78.86 158.55 223.28

TABLE 2 Case C-01 C-02 C-03 C-04 C-05 C-06 C-07 C-08 n₁₀ 2.1010 1.9972 1.8971 1.8903 1.7614 1.7825 1.7569 1.7277 k₁₀ 0.0000 0.1417 0.0932 0.1047 0.0933 0.0898 0.0868 0.0740 d₁₀(nm) 18.86 29.97 20.09 13.40 99.78 97.07 96.31 94.69 n₂₀ 2.3980 3.9849 1.8912 1.7190 1.8773 2.0041 1.7847 1.6779 k₂₀ 0.9577 0.5156 0.3589 0.2691 0.6361 0.3750 0.2610 0.2014 d₂₀(nm) 20.51 29.99 144.86 225.69 29.70 75.78 148.77 220.98 Case C-09 C-10 C-11 C-12 C-13 C-14 n₁₀ 1.7272 1.7147 1.7036 1.7000 1.7012 1.7028 k₁₀ 0.0744 0.0633 0.0666 0.0723 0.0708 0.0661 d₁₀(nm) 178.89 164.15 228.90 216.03 209.55 205.70 n₂₀ 2.1865 1.6838 2.1518 1.7881 1.7244 1.7099 k₂₀ 0.6947 0.1862 0.6409 0.3189 0.2345 0.1906 d₂₀(nm) 19.20 215.48 21.01 93.79 164.15 230.44 Case D-01 D-02 D-03 D-04 D-05 D-06 D-07 D-08 n₁₀ 2.0750 2.0118 1.8885 1.8806 1.7567 1.7300 1.7016 1.7036 k₁₀ 0.0000 0.1190 0.0999 0.1003 0.0923 0.0690 0.0665 0.0722 d₁₀(nm) 20.30 29.87 17.71 13.44 108.92 99.33 227.28 216.05 n₂₀ 2.4310 4.0092 1.7811 1.7062 2.0485 1.7059 2.1201 1.7959 k₂₀ 0.9366 0.5022 0.3211 0.2477 0.6631 0.1911 0.6392 0.3181 d₂₀(nm) 19.90 29.99 159.56 227.84 23.68 215.34 21.82 93.13 Case D-09 D-10 n₁₀ 1.7088 1.7083 k₁₀ 0.0700 0.0641 d₁₀(nm) 208.98 205.66 n₂₀ 1.7311 1.7076 k₂₀ 0.2343 0.1900 d₂₀(nm) 163.14 228.20 Case E-01 E-02 E-03 E-04 E-05 E-06 E-07 n₁₀ 2.0901 2.0375 1.8787 1.8780 1.7009 1.7204 1.7142 k₁₀ 0.0000 0.0819 0.1028 0.0706 0.0609 0.0677 0.0552 d₁₀(nm) 20.79 29.12 16.60 14.89 160.18 231.66 225.66 n₂₀ 2.4315 3.6552 1.7172 1.7467 1.6995 2.2460 1.7026 k₂₀ 0.9254 0.4960 0.2840 0.2361 0.1745 0.6523 0.1831 d₂₀(nm) 20.34 34.09 167.85 221.06 215.71 18.88 210.32

If any of the combinations of the values of [n₁₀, n₂₀, k₁₀, k₂₀, d₁₀, d₂₀] given above with which a minimum value of the reflectance is used, then the reflectance can be suppressed to 0.4% or less over the overall region of the incident angle corresponding to the pertaining numerical aperture NA of the exposure system. In other words, the combinations described above are effective combinations from the point of view that the reflectance can be made equal to or less than 0.4% even where the numerical aperture NA is smaller than the corresponding numerical aperture NA. Here, from among the combinations of the values of [n₁₀, n₂₀, k₁₀, k₂₀, d₁₀, d₂₀] given above, those combinations in the case of the numerical aperture NA=1.0 ([case A-01] to [case A-16]) are effective also where the numerical aperture NA is less than 1.0.

Meanwhile, those combinations in the case of the numerical aperture NA=1.1 ([case B-01] to [case B-16]) are effective also where the numerical aperture NA is equal to or less than 1.1, but is more preferable where the numerical aperture NA is more than 1.0 but equal to or less than 1.1. Furthermore, those combinations in the case of the numerical aperture NA=1.2 ([case C-01] to [case C-14]) are effective also where the numerical aperture NA is less than 1.2, but is more preferable where the numerical aperture NA is more than 1.1 but equal to or less than 1.2. Further, those combinations in the case of the numerical aperture NA=1.3 ([case D-01] to [case D-10]) are effective also where the numerical aperture NA is less than 1.3, but is more preferable where the numerical aperture NA is more than 1.2 but equal to or less than 1.3. Furthermore, those combinations in the case of the numerical aperture NA=1.4 ([case E-01] to [case E-07]) are effective also where the numerical aperture NA is less than 1.4, but is more preferable where the numerical aperture NA is more than 1.3 but equal to or less than 1.4.

A simulation was carried out with regard to the magnitude of variation of one of the variables of [n₁₀, n₂₀, k₁₀, k₂₀, d₁₀, d₂₀] in the combinations of the values of [n₁₀, n₂₀, k₁₀, k₂₀, d₁₀, d₂₀] given hereinabove while the remaining five variations were fixed when the reflectance exceeded 0.4%. As a result of the simulation, such variation permissible ranges indicated in Table 3 to Table 6 given below were obtained.

It is to be noted that, in the following description,

-   n_(1-MIN): minimum value of n₁₀ when the reflectance does not exceed     0.4%; -   n_(1-MAX): maximum value of n₁₀ when the reflectance does not exceed     0.4%; -   k_(1-MIN): minimum value of k₁₀ when the reflectance does not exceed     0.4%; -   k_(1-MAX): maximum value of k₁₀ when the reflectance does not exceed     0.4%; -   d_(1-MIN): minimum value of d₁₀ when the reflectance does not exceed     0.4%, -   d_(1-MAX): maximum value of d₁₀ when the reflectance does not exceed     0.4%; -   n_(2-MIN): minimum value of n₂₀ when the reflectance does not exceed     0.4%; -   n_(2-MAX): maximum value of n₂₀ when the reflectance does not exceed     0.4%; -   k_(2-MIN): minimum value of k₂₀ when the reflectance does not exceed     0.4%; -   k_(2-MAX): maximum value of k₂₀ when the reflectance does not exceed     0.4%; -   d_(2-MIN): minimum value of d₂₀ when the reflectance does not exceed     0.4%; -   d_(2-MAX): maximum value of d₂₀ when the reflectance does not exceed     0.4%.

Further, [case A-01] to [case A-16] are values for NA=1.0; [case B-01] to [case B-16] are values for NA=1.1; [case C-01] to [case C-14] are values for NA=1.2; [case D-01] to [case D-10] are values for NA=1.3; and [case E-01] to [case E-07] are values for NA=1.4.

TABLE 3 Case A-01 A-02 A-03 CA-04 A-05 A-06 A-07 n_(1-MAX) 2.2660 2.0526 1.9695 1.9914 1.8452 1.8547 1.8491 n_(1-MIN) 2.0674 1.8816 1.8041 1.8047 1.7221 1.7290 1.7286 k_(1-MAX) 0.1058 0.2476 0.1956 0.1790 0.1791 0.1675 0.1627 k_(1-MIN) 0.0000 0.0772 0.0266 0.0000 0.0475 0.0321 0.0280 d_(1-MAX)(nm) 19.64 35.17 31.59 26.35 108.00 108.98 109.36 d_(1-MIN)(nm) 13.49 25.28 16.46 11.04 81.48 80.83 80.19 n_(2-MAX) 2.4717 3.2954 2.1133 2.0045 1.8644 2.0858 2.0287 n_(2-MIN) 2.1929 2.9698 1.7768 1.6777 1.5730 1.7991 1.7335 k_(2-MAX) 1.1482 0.7497 0.6196 0.4975 0.7644 0.5849 0.5031 k_(2-MIN) 0.8579 0.4177 0.2781 0.2069 0.4915 0.2966 0.2049 d_(2-MAX)(nm) 25.55 42.99 ∞ ∞ 43.06 90.20 ∞ d_(2-MIN)(nm) 18.70 37.27 75.37 118.11 29.14 68.53 118.11 Case A-08 A-09 A-10 A-11 A-12 A-13 A-14 n_(1-MAX) 1.8363 1.8086 1.8145 1.8128 1.8044 1.8037 1.8053 n_(1-MIN) 1.7192 1.6900 1.6996 1.7051 1.7002 1.6700 1.6857 k_(1-MAX) 0.1158 0.1537 0.1529 0.1493 0.1428 0.1449 0.1450 k_(1-MIN) 0.0215 0.0304 0.0296 0.0310 0.0277 0.0218 0.0296 d_(1-MAX)(nm) 112.80 ∞ 193.81 194.11 ∞ ∞ ∞ d_(1-MIN)(nm) 79.23 146.42 145.32 144.88 144.10 147.03 206.52 n_(2-MAX) 1.9635 1.9536 2.0439 1.9727 1.9440 2.1270 2.0463 n_(2-MIN) 1.6573 1.6453 1.7648 1.6802 1.6149 1.7784 1.7598 k_(2-MAX) 0.4587 0.7451 0.5149 0.1493 0.4167 0.7867 0.4807 k_(2-MIN) 0.1553 0.4826 0.2558 0.0310 0.1340 0.4991 0.2325 d_(2-MAX)(nm) ∞ 36.88 89.13 ∞ ∞ 30.06 87.34 d_(2-MIN)(nm) 131.91 25.32 69.56 126.07 175.09 20.53 70.06 Case A-15 A-16 n_(1-MAX) 1.8030 1.7917 n_(1-MIN) 1.6894 1.6626 k_(1-MAX) 0.1411 0.1377 k_(1-MIN) 0.0354 0.0303 d_(1-MAX)(nm) ∞ ∞ d_(1-MIN)(nm) 206.86 147.71 n_(2-MAX) 1.9388 1.9597 n_(2-MIN) 1.6376 1.5656 k_(2-MAX) 0.4185 0.3989 k_(2-MIN) 0.1559 0.1211 d_(2-MAX)(nm) ∞ ∞ d_(2-MIN)(nm) 130.30 174.03

TABLE 4 Case B-01 B-02 B-03 B-04 B-05 B-06 B-07 n_(1-MAX) 2.2256 2.0568 1.9734 2.0082 1.8353 1.8462 1.8349 n_(1-MIN) 2.0472 1.9010 1.8223 1.8296 1.7330 1.7475 1.7473 k_(1-MAX) 0.0938 0.2244 0.1768 0.1635 0.1575 0.1496 0.1408 k_(1-MIN) 0.0000 0.0685 0.0175 0.0000 0.0495 0.0394 0.0374 d_(1-MAX)(nm) 20.80 34.77 29.62 23.26 112.91 109.31 108.27 d_(1-MIN)(nm) 14.63 25.76 16.06 10.49 87.82 87.00 86.56 n_(2-MAX) 2.4916 3.3028 2.0581 1.9623 1.9074 2.1009 1.9987 n_(2-MIN) 2.2319 3.0031 1.7577 1.6665 1.6538 1.8504 1.7392 k_(2-MAX) 1.1151 0.7242 0.5735 0.4524 0.7450 0.5318 0.4468 k_(2-MIN) 0.8400 0.4156 0.2710 0.2013 0.5085 0.2922 0.2015 d_(2-MAX)(nm) 24.36 42.69 ∞ ∞ 38.62 85.43 ∞ d_(2-MIN)(nm) 18.21 37.46 80.09 126.81 27.34 68.38 126.05 Case B-08 B-09 B-10 B-11 B-12 B-13 B-14 n_(1-MAX) 1.8028 1.8016 1.8041 1.7918 1.7729 1.7932 1.7879 n_(1-MIN) 1.7193 1.7039 1.7237 1.7262 1.6947 1.6903 1.7176 k_(1-MAX) 0.1323 0.1330 0.1299 0.1172 0.1176 0.1266 0.1177 k_(1-MIN) 0.0301 0.0370 0.0455 0.0534 0.0312 0.0317 0.0558 d_(1-MAX)(nm) 115.67 209.20 195.88 198.97 ∞ ∞ ∞ d_(1-MIN)(nm) 85.73 157.85 156.76 157.73 149.13 225.89 226.73 n_(2-MAX) 1.8971 2.0476 2.0364 1.8969 1.9046 2.4255 2.0020 n_(2-MIN) 1.6175 1.7703 1.8051 1.6706 1.5895 2.0733 1.8277 k_(2-MAX) 0.3623 0.7342 0.4294 0.3435 0.2910 0.8416 0.3876 k_(2-MIN) 0.1499 0.5070 0.2516 0.1729 0.1351 0.5371 0.2258 d_(2-MAX)(nm) ∞ 31.20 85.58 161.62 ∞ 21.50 87.70 d_(2-MIN)(nm) 181.56 22.38 72.33 139.39 187.96 15.15 76.00 Case B-15 B-16 n_(1-MAX) 1.7579 1.7716 n_(1-MIN) 1.6407 1.6465 k_(1-MAX) 0.1322 0.1321 k_(1-MIN) 0.0228 0.0178 d_(1-MAX)(nm) ∞ ∞ d_(1-MIN)(nm) 223.91 160.48 n_(2-MAX) 1.9149 2.1001 n_(2-MIN) 1.4543 1.4760 k_(2-MAX) 0.4261 0.4081 k_(2-MIN) 0.1424 0.1085 d_(2-MAX)(nm) ∞ ∞ d_(2-MIN)(nm) 129.53 143.86

TABLE 5 Case C-01 C-02 C-03 C-04 C-05 C-06 C-07 n_(1-MAX) 2.1902 2.0806 1.9757 1.9938 1.8213 1.8327 1.7995 n_(1-MIN) 2.0333 1.9400 1.8442 1.8243 1.7445 1.7698 1.7544 k_(1-MAX) 0.0791 0.2081 0.1538 0.1917 0.1313 0.1223 0.0982 k_(1-MIN) 0.0000 0.0680 0.0073 0.0023 0.0538 0.0533 0.0642 d_(1-MAX)(nm) 22.17 34.24 27.46 20.29 118.37 109.28 111.91 d_(1-MIN)(nm) 16.20 26.95 16.03 9.40 96.05 94.62 95.76 n_(2-MAX) 2.5150 4.1060 2.0062 1.8367 1.9517 2.0899 1.8293 n_(2-MIN) 2.2758 3.8579 1.7470 1.5737 1.7548 1.9035 1.6980 k_(2-MAX) 1.0902 0.6644 0.5181 0.3688 0.7101 0.4366 0.3015 k_(2-MIN) 0.8269 0.4039 0.2637 0.1833 0.5274 0.2899 0.2021 d_(2-MAX)(nm) 23.39 31.19 ∞ ∞ 33.13 81.59 161.61 d_(2-MIN)(nm) 17.92 28.87 85.53 141.88 25.36 70.00 146.51 Case C-08 C-09 C-10 C-11 C-12 C-13 C-14 n_(1-MAX) 1.7711 1.7845 1.7573 1.7333 1.7203 1.7336 1.7514 n_(1-MIN) 1.7097 1.7167 1.6822 1.6243 1.6387 1.6472 1.6539 k_(1-MAX) 0.1152 0.1077 0.1011 0.1086 0.1103 0.1181 0.1191 k_(1-MIN) 0.0321 0.0488 0.0264 0.0356 0.0460 0.0368 0.0268 d_(1-MAX)(nm) 114.36 218.45 ∞ ∞ 227.26 237.88 ∞ d_(1-MIN)(nm) 89.11 175.03 147.22 181.97 190.09 179.63 173.04 n_(2-MAX) 1.7201 2.2837 1.7321 2.3031 1.9012 1.8497 1.8964 n_(2-MIN) 1.5934 2.0604 1.6046 2.0795 1.7532 1.6568 1.5385 k_(2-MAX) 0.2464 0.7527 0.2137 0.7063 0.3281 0.3333 0.3179 k_(2-MIN) 0.1479 0.5549 0.1380 0.5137 0.2264 0.1529 0.1170 d_(2-MAX)(nm) ∞ 21.11 235.37 24.52 111.38 ∞ ∞ d_(2-MIN)(nm) 196.47 16.79 195.03 19.07 89.55 150.63 157.43

TABLE 6 Case D-01 D-02 D-03 D-04 D-05 D-06 D-07 n_(1−MAX) 2.1541 2.0844 1.9589 1.9713 1.7997 1.7599 1.7325 n_(1−MIN) 2.0215 1.9638 1.8538 1.8291 1.7557 1.7290 1.6697 k_(1−MAX) 0.0610 0.1705 0.1459 0.1729 0.0954 0.0744 0.1071 k_(1−MIN) 0.0000 0.0518 0.0187 0.0078 0.0655 0.0522 0.0350 d_(1−MAX)(nm) 23.54 33.58 23.82 19.76 125.01 114.51 249.66 d_(1−MIN)(nm) 18.03 27.42 15.13 10.09 108.67 98.99 206.91 n_(2−MAX) 2.5291 4.1084 1.8635 1.7809 2.0547 1.7114 2.2630 n_(2−MIN) 2.3203 3.9019 1.6624 1.5899 1.9572 1.6501 2.0448 k_(2−MAX) 1.0610 0.6325 0.4092 0.3139 0.6691 0.1929 0.7020 k_(2−MIN) 0.8178 0.4040 0.2433 0.1776 0.5710 0.1524 0.5119 d_(2−MAX)(nm) 22.43 30.97 ∞ ∞ 23.86 219.55 25.26 d_(2−MIN)(nm) 17.62 29.03 129.86 149.42 21.22 205.88 19.68 Case D-08 D-09 D-10 n_(1−MAX) 1.7213 1.7343 1.7487 n_(1−MIN) 1.6816 1.6905 1.6839 k_(1−MAX) 0.1083 0.1002 0.0965 k_(1−MIN) 0.0475 0.0408 0.0326 d_(1−MAX)(nm) 226.44 234.14 ∞ d_(1−MIN)(nm) 203.38 198.02 187.04 n_(2−MAX) 1.9107 1.8583 1.8700 n_(2−MIN) 1.7644 1.6757 1.5497 k_(2−MAX) 0.3809 0.3287 0.3066 k_(2−MIN) 0.2256 0.1573 0.1188 d_(2−MAX)(nm) 110.64 ∞ ∞ d_(2−MIN)(nm) 89.45 150.12 160.78 Case E-01 E-02 E-03 E-04 E-05 E-06 E-07 n_(1−MAX) 2.1532 2.0916 1.9323 1.9461 1.7131 1.7346 1.7449 n_(1−MIN) 2.0485 1.9946 1.8625 1.8482 1.6965 1.7142 1.7015 k_(1−MAX) 0.0301 0.1157 0.1287 0.1125 0.0797 0.0791 0.0776 k_(1−MIN) 0.0000 0.0234 0.0358 0.0000 0.0529 0.0480 0.0279 d_(1−MAX)(nm) 23.53 31.97 21.01 20.40 168.49 241.66 269.84 d_(1−MIN)(nm) 19.45 27.24 15.35 12.65 156.71 227.75 215.83 n_(2−MAX) 2.4915 3.7301 1.7470 1.7894 1.7056 2.3315 1.8141 n_(2−MIN) 2.3369 3.5977 1.6335 1.6492 1.6786 2.2068 1.6257 k_(2−MAX) 1.0253 0.5706 0.3145 0.2771 0.1981 0.6941 0.2591 k_(2−MIN) 0.8408 0.4125 0.2297 0.1801 0.1502 0.5188 0.1258 d_(2−MAX)(nm) 22.48 35.05 ∞ ∞ 219.96 20.91 ∞ d_(2−MIN)(nm) 18.31 33.41 144.47 152.04 200.15 17.96 186.01

The combinations of the values of [n₁₀, n₂₀, k₁₀, k₂₀, d₁₀, d₂₀] are combinations which minimize the reflectances over the overall region of the incident angle corresponding to the corresponding numerical aperture NA of the exposure system. In particular, where the evaluation function for the minimization is represented by f, the evaluation function f is a function of n₁₀, n₂₀, k₁₀, k₂₀, d₁₀ and d₂₀, and the combinations which minimize the f(n₁₀, n₂₀, k₁₀, k₂₀, d₁₀, d₂₀) is such combinations of the values of [n₁₀, n₂₀, k₁₀, k₂₀, d₁₀, d₂₀] as given hereinabove. In other words, the evaluation function f is minimized with such combinations of the values of [n₁₀, n₂₀, k₁₀, k₂₀, d₁₀, d₂₀] as given hereinabove.

Generally, where the evaluation function f(x_(i)) (i=0, 1, 2, . . . , n) exhibits a minimum value at x_(i)=x_(i-MIN), in the proximity of the minimum value, the evaluation function f(x_(i)) can be represented by the following expression (1): f(x _(i))=Σa _(i)(x _(i) −x _(i-MIN))² +b  (1) In other words, the evaluation function f(x_(i)) can be approximated with a quadratic function. It is to be noted that the symbol “Σ” signifies the sum total for i=0, 1, 2, . . . , n. This similarly applies also to the expression (2).

In this instance, a condition that the evaluation function f(x_(i)) is smaller than a fixed number c which is greater than b can be represented by an elliptic function of the following expression (2): Σ(x _(i)-x _(1-MIN))²/(x _(i-c)-x _(i-MIN))₂≦1  (2) where x_(i-c) is the value of x_(i) with which f(x_(i))=c is obtained when all of the other variables are fixed while only x_(i) is varied.

Therefore, if n₁₀, n₂₀, k₁₀, k₂₀, d₁₀ and d₂₀ which satisfy the following expression (3) using values of n_(1-MAX), n_(1-MIN), k_(1-MAX), k_(1-MIN), d_(1-MAX), d_(1-MIN), n_(2-MAX), n_(2-MIN), k_(2-MAX), k_(2-MIN), d_(2-MAX) and d_(2-MIN) which are values with which the reflectance of 0.4% is obtained when only one of the variables is varied while the other variables are fixed are adopted, then the reflectance does not exceed 0.4%. {(n ₁-n ₁₀)/(n _(1m)-n ₁₀)}²+{(k ₁-k ₁₀)/(k _(1m)-k ₁₀)}²+{(d ₁-d ₁₀)/(d _(1m)-d ₁₀)}²+{(n ₂-n ₂₀)/(n _(2m)-n ₂₀)}²+{(k ₂-k ₂₀)/(k _(2m)-k ₂₀)}²+{(d ₂-d ₂₀)/(d _(2m)-d ₂₀)}²≦1  (3) where n_(1m), k_(1m), d_(1m), n_(2m), k_(2m) and d_(2m) assume the following values: n_(1m): for n₁≧n₁₀, n_(1-MAX), for n₁<n₁₀, n_(1-MIN) k_(1m): for k₁≧k₁₀, k_(1-MAX), for k₁<k₁₀, k_(1-MIN) d_(1m): for d₁≧d₁₀, d_(1-max), for d₁<d₁₀, d_(1-MIN) n_(2m): for n₂≧n₂₀, n_(2-MAX), for n₂<n₂₀, n_(2-MIN) k_(2m): for k₂≧k₂₀, k_(2-MAX), for k₂<k₂₀, k_(2-MIN) d_(2m): for d₂≧d₂₀, d_(2-MAX), for d₂<d₂₀, d_(2-MIN)

It is to be noted that the reason why the values of n_(1m), k_(1m), d_(1m), n_(2m), k_(2m) and d_(2m) are separated depending upon the relationship in magnitude where n₁, n₂, k₁, k₂, d₁ and d₂ are compared with n₁₀, n₂₀, k₁₀, k₂₀, d₁₀ and d₂₀, respectively, is that, since n_(1-MAX)-n₁₀=n₁₀-n_(1-MIN) k_(1-MAX)-k₁₀=k₁₀-k_(1-MIN) d_(1-MAX)-d₁₀=d₁₀-d_(1-MIN) n_(2-MAX)-n₂₀=n₂₀-n_(2-MIN) k_(2-MAX)-k₂₀=k₂₀-k_(2-MIN) d_(2-MAX)-d₂₀=d₂₀-d_(2-MIN) are not always satisfied, the definition of an ellipsoid defined by the expression (2) given above is separated depending upon the relationship in magnitude when n₁, n₂, k₁, k₂, d₁ and d₂ are compared with n₁₀, n₂₀, k₁₀, k₂₀, d₁₀ and d₂₀, respectively. In other words, this is because the curvature of an ellipsoid exhibits different values, for example, whether n₁≧n₁₀ or n₁<n₁₀, and this similarly applies also to k₁₀, d₁₀, n₂₀, k₂₀ and d₂₀.

Thus, where, as a combination of values of [n₁₀, n₂₀, k₁₀, k₂₀, d₁₀, d₂₀],

-   for NA≦1.0, one of the case [1-01] to the case [1-16], -   for 1.0<NA≦1.1, one of the case [2-01] to the case [2-16], -   for 1.1<NA≦1.2, one of the case [3-01] to the case [3-14], -   for 1.2<NA≦1.3, one of the case [4-01] to the case [4-10], or -   for 1.3<NA≦1.4, one of the case [5-01] to the case [5-07] -   is adopted, it is guaranteed that the reflectance does not exceed     0.4%. Besides, where -   the value of n_(1m) for the pertaining case is adopted based on the     relationship in magnitude between n₁ and n₁₀, -   the value of k_(1m) for the pertaining case is adopted based on the     relationship in magnitude between k₁ and k₁₀, -   the value of d_(1m) for the pertaining case is adopted based on the     relationship in magnitude between d₁ and d₁₀, -   the value of n_(2m) for the pertaining case is adopted based on the     relationship in magnitude between n₂ and n₂₀, -   the value of k_(2m) for the pertaining case is adopted based on the     relationship in magnitude between k₂ and k₂₀, and -   the value of d_(2m) for the pertaining case is adopted based on the     relationship in magnitude between d₂ and d₂₀, if -   n₁ is within the range between the maximum value (n_(1-MAX)) and the     minimum value (n_(1-MIN)) of n_(1m) for the pertaining case, -   k₁ is within the range between the maximum value (k_(1-MAX)) and the     minimum value (k_(1-MIN)) of k_(1m) for the pertaining case, -   d₁ is within the range between the maximum value (d_(1-MAX)) and the     minimum value (d_(1-MIN)) of d_(1m) for the pertaining case, -   n₂ is within the range between the maximum value (n_(2-MAX)) and the     minimum value (n_(2-MIN)) of n_(2m) for the pertaining case, -   k₂ is within the range between the maximum value (k_(2-MAX)) and the     minimum value (k_(2-MIN)) of k_(2m) for the pertaining case, and -   d₂ is within the range between the maximum value (d_(2-MAX)) and the     minimum value (d_(2-MIN)) of d_(2m) for the pertaining case,     then it is guaranteed that the reflectance of the antireflection     film from the silicon semiconductor substrate does not exceed 0.4%.     As a result, a good resist pattern can be obtained.

In other words, where a six-dimensional ellipsis whose center is given by (n₁₀, n₂₀, k₁₀, k₂₀, d₁₀, d₂₀) and whose diameter is defined by six variables of (n₁, k₁, d₁, n₂, k₂, d₂) which are absolute values of (n_(1m)-n₁₀), (k_(1m)-k₁₀), (d_(1m)-d₁₀), (n_(2m)-n₂₀), (k_(2m)-k₂₀), (d_(2m)-d₂₀), respectively, is assumed, if a combination of arbitrary values of n₁, k₁, d₁, n₂, k₂, d₂ within the range of the inside of the ellipsis is selected, then the reflectance of the antireflection film can be suppressed to 0.4% or less.

EXAMPLES

Two-layer antireflection films having reflectances and film thicknesses indicated in Table 7 and hereinafter described were formed on the surface of a silicon semiconductor substrate by a plasma enhanced CVD method disclosed in Japanese Patent 2001-242630, K. Babich et al., Proceedings of SPIE 2003, 5039, 152 and so forth.

It is to be noted that the plasma enhanced CVD method is a film formation method which is carried out in a parallel electrode reactor as explained in detail in the documents mentioned above, and a silicon semiconductor substrate is placed on one of the electrodes. A negative bias is applied from the electrode to the silicon semiconductor substrate, and layers having various values of the complex refractive index can be formed by controlling the pressure in the reactor, the type (tetramethylsilane, trimethylsilane, tetramethyltetrasiloxane, tetramethylgermane, oxygen or the like) and the flow rate of a reaction precursor to be introduced into the reactor and the substrate temperature.

It is to be noted that, in Table 7, examples 1 to 7 represent antireflection films which satisfy the conditions of the present invention while a comparative example 1 and comparative examples 2 to 4 represent antireflection films for comparison which do not satisfy the conditions of the present invention.

More particularly, the examples 1 and 6 are antireflection films which satisfy the conditions of the present invention where the numerical aperture NA of the exposure system is within the range of NA≦1.0, and the examples 2 and 7 are antireflection films which satisfy the conditions of the present invention where the numerical aperture NA of the exposure system is within the range of 1.0<NA≦1.1. Meanwhile, the example 3 is an antireflection film which satisfies the conditions of the present invention where the numerical aperture NA of the exposure system is within the range of 1.1<NA≦1.2, and the example 4 is an antireflection film which satisfies the conditions of the present invention where the numerical aperture NA of the exposure system is within the range of 1.2<NA≦1.3. Further, the example 5 is an antireflection film which satisfies the conditions of the present invention where the numerical aperture NA of the exposure system is within the range of 1.3<NA≦1.4. In all of the antireflection films of the examples 1 to 7 and the comparative examples 1 to 4 described below, the upper layer and the lower layer are formed from a material of SiCOH. It is to be noted that the complex refractive index of each film was measured using an ellipsometer by SOPRA.

The comparative example 1 is an antireflection film which satisfies none of the conditions of the present invention where the numerical aperture NA of the exposure system is within the range of NA≦1.0 and the conditions of the present invention where the numerical aperture NA of the exposure system is within the range of 1.0<NA≦1.1. Meanwhile, the comparative examples 2, 3 and 4 are antireflection films which do not satisfy the conditions of the present invention where the numerical aperture NA of the exposure system is within the ranges of 1.1<NA≦1.2, 1.2<NA≦1.3, and 1.3<NA≦1.4, respectively.

A photoresist ARX2014J by JSR was spin coated to a film thickness of 100 nm as a resist layer on the two-layer antireflection film of the examples 1 to 7 and the comparative examples 1 to 4, and then a baking process was performed for 60 seconds at 20° C. Then, a top coat material TCX001 by JSR was spin coated to a film thickness of 30 nm. Thereafter, a baking process was performed for the entire films for 30 seconds at 100° C.

Any of the samples produced in such a manner as described above was exposed by a two-beam interference exposure apparatus. The two-beam interference exposure apparatus uses an ArF excimer laser as a light source and includes a prism having a triangular or pentagonal cross section and disposed on a light path of the laser. The sample was disposed below the lower face of the prism such that the distance between the sample and the lower face of the prism was 1 mm. For example, where a prism having a triangular cross section is used, a vertex of the prism is disposed at a central location of the light path of the laser, and the face of the prism opposing to the vertex is determined as the lower face. If a laser beam is illuminated on the prism from above the prism toward the lower face of the prism, then the laser beam incident to the two side faces of the prism is refracted by the side faces relying upon the angles between the side faces and the incident laser beam and changes the direction of the light path thereof so that it is split into two laser beams. The two laser beam portions from the two side faces having different advancing directions intersect and interfere with each other on the lower face of the prism thereby to form a periodic optical intensity distribution on the sample. Consequently, the resist layer can be sensitized.

Then, the angles between the side faces of the prism and the incident laser beam can be varied by using various prisms having various different vertical angles as the prism, and an optical intensity distribution having an arbitrary pitch can be obtained on the sample below the lower face of the prism. Since the resist layer is resolved in accordance with the optical intensity distribution, if only the shape of the prism is changed in the exposure method, then a line and space pattern of an arbitrary pitch can be obtained.

Liquid immersion exposure in which water was used as the liquid for liquid immersion by introducing water into the gap of 1 mm between the sample and the prism making use of a capillarity.

Further, five different prisms were prepared for the two-beam interference exposure test. The five prisms have numerical apertures NA of 0.75, 1.06, 1.15, 1.22 and 1.39.

For the examples 1 and 6, the prism whose numerical aperture NA is 0.75 was used for the exposure; for the examples 2 and 7, the prism whose numerical aperture NA is 1.06 was used; for the example 3, the prism whose numerical aperture NA is 1.15 was used; for the example 4, the prism whose numerical aperture NA is 1.22 was used; and for the example 5, the prism whose numerical aperture NA is 1.39 was used.

Meanwhile, for the comparative example 1, the prism whose numerical aperture NA is 1.06 was used for the exposure; for the comparative example 2, the prism whose numerical aperture NA is 1.15 was used; for the comparative example 3, the prism whose numerical aperture NA is 1.22 was used; and for the comparative example 4, the prism whose numerical aperture NA is 1.39 was used.

A baking process was applied for 90 seconds at 120° C. to the samples after the exposure, and then development was performed with a standard developer made of 2.38% TMAH (tetramethyl ammonium hydroxide) to produce samples for resist pattern observation. The shape observation of the resist layer was performed by dividing the silicon semiconductor substrate and observing the cross section using a scanning electron microscope.

As a result of the observation, any sample whose resist pattern has a good rectangular cross section is indicated by a round mark “o” while any sample whose resist pattern does not have a good rectangular cross section is indicated by a cross mark “x” in Table 7.

TABLE 7 Upperlayer Lowerlayer Double Upperlayer Double Lowerlayer Refractive Film refractive Film Index N₁ thickness Index N₂ thickness Conversion N₁ = n₁ − k₁i (nm) N₂ = n₂ − k₂i (nm) numerical Sectional Case n₁ k₁ d₁ n₂ k₂ d₂ aperture pattern Example 1 A-03 1.88 0.10 23 1.95 0.40 135 0.75 ◯ Example 2 B-03 1.88 0.10 21 1.95 0.40 135 1.06 ◯ Example 3 C-03 1.88 0.10 21 1.89 0.36 145 1.15 ◯ Example 4 D-03 1.90 0.10 18 1.79 0.32 160 1.22 ◯ Example 5 E-03 1.88 0.10 17 1.65 0.28 168 1.39 ◯ Example 6 A-16 1.72 0.06 220  1.73 0.20 207 0.75 ◯ Example 7 B-16 1.72 0.06 265  1.73 0.20 220 1.06 ◯ Comparative — 1.90 0.10 31 1.60 0.40 135 1.06 X example 1 Comparative — 1.80 0.10 30 1.55 0.40 135 1.15 X example 2 Comparative — ″ ″ ″ ″ ″ ″ 1.22 X example 3 Comparative — ″ ″ ″ ″ ″ ″ 1.39 X example 4

As apparently seen from Table 7, the antireflection films of a two-layer configuration to which the present invention is applied have a better cross sectional shape of a resist than the antireflection films of a two-layer configuration to which the present invention is not applied.

In this manner, where an antireflection film of a two-layer configuration which has a double refractive index and a film thickness which are individually within particular ranges is formed between a resist layer and the surface of a silicon semiconductor substrate by applying the present invention, the reflectance from the silicon semiconductor substrate in the antireflection film corresponding to the numerical aperture NA of the exposure system which is within a fixed range can be reduced. Consequently, a good resist pattern can be obtained.

It is to be noted that, while, in the examples described above, an antireflection film of a two-layer configuration formed by a plasma enhanced CVD method is described as an example, according to the present invention, the antireflection film of a two-layer configuration is not limited to this but may be formed, for example, by a spin coating method or any other method.

Semiconductor devices were fabricated using the antireflection films of a two-layer configuration of the present invention. It is to be noted that a phase shift mask was used as the exposure mask while an ArF excimer laser (wavelength λ: 193 nm) was used as the light source for exposure light, and a zone illumination method was adopted. Further, the surface of the resist layer was covered with a water layer. Then, it was verified whether or not a desired pattern could be formed on the resist layer without any fluctuation in line width or shape. As a result, it was found that, in any case, a desired pattern could be formed on the resist layer without any fluctuation in line width or shape. Besides, in any case, the reflectance was equal to or less than 0.4.

In particular, formation of an element isolation region having a trench structure was performed. More particularly, an antireflection film having a two-layer structure was formed on a silicon semiconductor substrate, and a resist layer was formed on the antireflection film and then exposed and developed to obtain a patterned resist layer. Then, the silicon semiconductor substrate was etched to a predetermined depth by an RIE method using the patterned resist layer as an etching mask to form a trench on the silicon semiconductor substrate. Thereafter, an insulator film is formed on the overall face of the silicon semiconductor substrate including the trench, and then the insulator film on the surface of the silicon semiconductor substrate was removed to obtain an element isolation region having a trench structure wherein the isolation film is embedded in the trench formed on the silicon semiconductor substrate.

While preferred examples of the present invention are described above, the present invention is not limited to the specific examples, but the configuration of the antireflection film and the film thicknesses and the complex refraction indices of the layers which form the antireflection film in the examples are for illustrative purposes only and can be altered suitably. 

1. A method for patterning a resist layer comprising the steps of: providing a silicon semiconductor substrate; providing a resist layer above the semiconductor substrate; providing an antireflection film between a surface of the silicon semiconductor substrate and said resist layer; and exposing the resist layer to light having a wavelength of 190 nm to 195 nm via a system having a numerical aperture equal to or less than 1, wherein, said antireflection film includes an upper layer having a complex refractive index N₁ equal to n₁-k₁i and a film thickness d₁, and a lower layer having a complex refractive index N₂ equal to n₂-k₂i and a film thickness d₂, said upper layer and said lower layer configured such that the values of n₁₀, k₁₀, d₁₀, n₂₀, k₂₀, d₂₀, n₁, k₁, d₁, n₂, k₂ and d₂ satisfy a Formula 1 {(n ₁-n ₁₀)/(n _(1m)-n ₁₀)}²+{(k ₁-k ₁₀)/(k _(1m)-k ₁₀)}²+{(d ₁-d ₁₀)/(d _(1m)-d ₁₀)}²+{(n ₂-n ₂₀) /(n _(2m)-n ₂₀)}²+{(k ₂-k ₂₀)/(k _(2m)-k ₂₀)}²+{(d ₂-d ₂₀)/(d _(2m)-d ₂₀)}²≦1,   Formula 1: the values of n₁₀, k₁₀, d₁₀, n₂₀, k₂₀, d₂₀, n₁, k₁, d₁, n₂, k₂ and d₂ are defined by one of cases [0-01] to [1-16] in Tables 1-1 through 1-4, (a) a value of n_(1m) in the pertaining case is adopted based on a relationship in magnitude between n₁ and n₁₀; (b) a value of k_(1m) in the pertaining case is adopted based on a relationship in magnitude between k₁ and k₁₀; (c) a value of d_(1m) in the pertaining case is adopted based on a relationship in magnitude between d₁ and d₁₀; (d) a value of n_(2m) in the pertaining case is adopted based on a relationship in magnitude between n₂ and n₂₀; (e) a value of k_(2m) in the pertaining case is adopted based on a relationship in magnitude between k₂ and k₂₀; and (f) a value of d_(2m) in the pertaining case is adopted based on a relationship in magnitude between d₂ and d₂₀, and Tables 1-1 through 1-4 are: TABLE 1-1 Case 1-01 1-02 1-03 1-04 1-05 n₁₀ 2.1616 1.9575 1.8783 1.8886 1.7671 k₁₀ 0.0031 0.1578 0.1120 0.0828 0.0972 d₁₀ (nm) 16.39 29.70 22.79 17.43 89.65 n₂₀ 2.3326 3.1421 1.9535 1.8540 1.7266 k₂₀ 0.9955 0.5540 0.3987 0.3157 0.6265 d₂₀ (nm) 21.81 39.99 133.42 201.01 35.79 for n₁ ≧ 2.2660 2.0526 1.9695 1.9914 1.8452 n₁₀, n_(1m) = for n₁ < 2.0674 1.8816 1.8041 1.8047 1.7221 n₁₀, n_(1m) = for k₁ ≧ 0.1058 0.2476 0.1956 0.1790 0.1791 k₁₀, k_(1m) = for k₁ < 0.0000 0.0772 0.0266 0.0000 0.0475 k₁₀, k_(1m) = for d₁ ≧ 19.64 35.17 31.59 26.35 108.00 d₁₀, d_(1m) (nm) = for d₁ < 13.49 25.28 16.46 11.04 81.48 d₁₀, d_(1m) (nm) = for n₂ ≧ 2.4717 3.2954 2.1133 2.0045 1.8644 n₂₀, n_(2m) = for n₂ < 2.1929 2.9698 1.7768 1.6777 1.5730 n₂₀, n_(2m) = for k₂ ≧ 1.1482 0.7497 0.6196 0.4975 0.7644 k₂₀, k_(2m) = for k₂ < 0.8579 0.4177 0.2781 0.2069 0.4915 k₂₀, k_(2m) = for d₂ ≧ 25.55 42.99 ∞ ∞ 43.06 d₂₀, d_(2m) (nm) = for d₂ < 18.70 37.27 75.37 118.11 29.14 d₂₀, d_(2m) (nm) =

TABLE 1-2 Case 1-06 1-07 1-08 1-09 1-10 n₁₀ 1.7783 1.7756 1.7637 1.7297 1.7402 k₁₀ 0.0854 0.0827 0.0788 0.0695 0.0705 d₁₀ (nm) 90.09 89.16 88.60 159.09 157.00 n₂₀ 1.9451 1.8813 1.8074 1.8027 1.9115 k₂₀ 0.4110 0.2980 0.2358 0.6176 0.3647 d₂₀ (nm) 78.70 136.86 201.53 30.94 79.38 for n₁ ≧ 1.8547 1.8491 1.8363 1.8086 1.8145 n₁₀, n_(1m) = for n₁ < 1.7290 1.7286 1.7192 1.6900 1.6996 n₁₀, n_(1m) = for k₁ ≧ 0.1675 0.1627 0.1158 0.1537 0.1529 k₁₀, k_(1m) = for k₁ < 0.0321 0.0280 0.0215 0.0304 0.0296 k₁₀, k_(1m) = for d₁ ≧ 108.98 109.36 112.80 ∞ 193.81 d₁₀, d_(1m) (nm) = for d₁ < 80.83 80.19 79.23 146.42 145.32 d₁₀, d_(1m) (nm) = for n₂ ≧ 2.0858 2.0287 1.9635 1.9536 2.0439 n₂₀, n_(2m) = for n₂ < 1.7991 1.7335 1.6573 1.6453 1.7648 n₂₀, n_(2m) = for k₂ ≧ 0.5849 0.5031 0.4587 0.7451 0.5149 k₂₀, k_(2m) = for k₂ < 0.2966 0.2049 0.1553 0.4826 0.2558 k₂₀, k_(2m) = for d₂ ≧ 90.20 ∞ ∞ 36.88 89.13 d₂₀, d_(2m) (nm) = for d₂ < 68.53 118.11 131.91 25.32 69.56 d₂₀, d_(2m) (nm) =

TABLE 1-3 Case 1-11 1-12 1-13 1-14 1-15 n₁₀ 1.7416 1.7346 1.7204 1.7293 1.7290 k₁₀ 0.0723 0.0700 0.0573 0.0638 0.0672 d₁₀ (nm) 154.81 154.48 226.55 221.51 219.00 n₂₀ 1.8276 1.7635 1.9505 1.9167 1.7992 k₂₀ 0.2602 0.2082 0.6496 0.3426 0.2416 d₂₀ (nm) 140.99 205.63 25.08 78.00 142.68 for n₁ ≧ 1.8128 1.8044 1.8037 1.8053 1.8030 n₁₀, n_(1m) = for n₁ < 1.7051 1.7002 1.6700 1.6857 1.6894 n₁₀, n_(1m) = for k₁ ≧ 0.1493 0.1428 0.1449 0.1450 0.1411 k₁₀, k_(1m) = for k₁ < 0.0310 0.0277 0.0218 0.0296 0.0354 k₁₀, k_(1m) = for d₁ ≧ 194.11 ∞ ∞ ∞ ∞ d₁₀, d_(1m) (nm) = for d₁ < 144.88 144.10 147.03 206.52 206.86 d₁₀, d_(1m) (nm) = for n₂ ≧ 1.9727 1.9440 2.1270 2.0463 1.9388 n₂₀, n_(2m) = for n₂ < 1.6802 1.6149 1.7784 1.7598 1.6376 n₂₀, n_(2m) = for k₂ ≧ 0.1493 0.4167 0.7867 0.4807 0.4185 k₂₀, k_(2m) = for k₂ < 0.0310 0.1340 0.4991 0.2325 0.1559 k₂₀, k_(2m) = for d₂ ≧ ∞ ∞ 30.06 87.34 ∞ d₂₀, d_(2m) (nm) = for d₂ < 126.07 175.09 20.53 70.06 130.30 d₂₀, d_(2m) (nm) =

TABLE 1-4 Case 1-16 n₁₀ 1.7210 k₁₀ 0.0630 d₁₀ (nm) 220.18 n₂₀ 1.7329 k₂₀ 0.1973 d₂₀ (nm) 207.16 for n₁ ≧ 1.7917 n₁₀, n_(1m) = for n₁ < 1.6626 n₁₀, n_(1m) = for k₁ ≧ 0.1377 k₁₀, k_(1m) = for k₁ < 0.0303 k₁₀, k_(1m) = for d₁ ≧ ∞ d₁₀, d_(1m) (nm) = for d₁ < 147.71 d₁₀, d_(1m) (nm) = for n₂ ≧ 1.9597 n₂₀, n_(2m) = for n₂ < 1.5656 n₂₀, n_(2m) = for k₂ ≧ 0.3989 k₂₀, k_(2m) = for k₂ < 0.1211 k₂₀, k_(2m) = for d₂ ≧ ∞ d₂₀, d_(2m) (nm) = for d₂ < 174.03. d₂₀, d_(2m) (nm) =


2. The patterning method according to claim 1, wherein the film thickness d₁ of said upper layer satisfies d₁ ≦250, and the film thickness d₂ of said lower layer satisfies d₂ ≦250.
 3. The patterning method according to claim 1, wherein the resist layer has a refractive index of 1.60 to 1.80.
 4. A method for patterning a resist layer comprising the steps of: providing a silicon semiconductor substrate; providing a resist layer above the semiconductor substrate; providing an antireflection film between a surface of the silicon semiconductor substrate and said resist layer; and exposing the resist layer to light having a wavelength of 190 nm to 195 nm via a system having a numerical aperture of more than 1.0 but less than or equal to 1.1, wherein, said antireflection film includes an upper layer having a complex refractive index N₁ equal to n₁-k₁i and a film thickness d₁, and a lower layer having a complex refractive index N₂ equal to n₂-k₂i and a film thickness d₂; said upper layer and said lower layer configured such that the values of n₁₀, k₁₀, d₁₀, n₂₀, k₂₀, d₂₀] n₁, k₁, d₁, n₂, k₂ and d₂ satisfy a Formula 1 {(n ₁-n ₁₀)/(n _(1m)-n ₁₀)}²+{(k ₁-k ₁₀)/(k _(1m)-k ₁₀)}²+{(d ₁-d ₁₀)/(d _(1m)-d ₁₀)}²+{(n ₂-n ₂₀) /(n _(2m)-n ₂₀)}²+{(k ₂-k ₂₀)/(k _(2m)-k ₂₀)}²+{(d ₂-d ₂₀)/(d _(2m)-d ₂₀)}²≦1,   Formula 1: the values of n₁₀, k₁₀, d₁₀, n₂₀, k₂₀, d₂₀] n₁, k₁, d₁, n₂, k₂ and d₂ are defined by one of cases [2-01] to [2-16] in Tables 2-1 through 2-4, (a) a value of n_(1m) in the pertaining case is adopted based on a relationship in magnitude between n₁ and n₁₀; (b) a value of k_(1m) in the pertaining case is adopted based on a relationship in magnitude between k₁ and k₁₀; (c) a value of d_(1m) in the pertaining case is adopted based on a relationship in magnitude between d₁ and d₁₀;(d) a value of n_(2m) in the pertaining case is adopted based on a relationship in magnitude between n₂ and n₂₀; (e) a value of k_(2m) in the pertaining case is adopted based on a relationship in magnitude between k₂ and k₂₀; and (f) a value of d_(2m) in the pertaining case is adopted based on a relationship in magnitude between d₂ and d₂₀, and Tables 2-1 through 2-4 are: TABLE 2-1 Case 2-01 2-02 2-03 2-04 2-05 n₁₀ 2.1270 1.9689 1.8874 1.9059 1.7643 k₁₀ 0.0000 0.1461 0.1027 0.0744 0.0947 d₁₀ (nm) 17.47 26.67 21.38 15.49 94.08 n₂₀ 2.3628 3.1616 1.9199 1.8297 1.7955 k₂₀ 0.9776 0.5440 0.3802 0.2998 0.6320 d₂₀ (nm) 21.04 39.98 139.31 207.65 32.98 for n₁ ≧ 2.2256 2.0568 1.9734 2.0082 1.8353 n₁₀, n_(1m) = for n₁ < 2.0472 1.9010 1.8223 1.8296 1.7330 n₁₀, n_(1m) = for k₁ ≧ 0.0938 0.2244 0.1768 0.1635 0.1575 k₁₀, k_(1m) = for k₁ < 0.0000 0.0685 0.0175 0.0000 0.0495 k₁₀, k_(1m) = for d₁ ≧ 20.80 34.77 29.62 23.26 112.91 d₁₀, d_(1m) (nm) = for d₁ < 14.63 25.76 16.06 10.49 87.82 d₁₀, d_(1m) (nm) = for n₂ ≧ 2.4916 3.3028 2.0581 1.9623 1.0974 n₂₀, n_(2m) = for n₂ < 2.2319 3.0031 1.7577 1.6665 1.6538 n₂₀, n_(2m) = for k₂ ≧ 1.1151 0.7242 0.5735 0.4524 0.7450 k₂₀, k_(2m) = for k₂ < 0.8400 0.4156 0.2710 0.2013 0.5085 k₂₀, k_(2m) = for d₂ ≧ 24.36 42.69 ∞ ∞ 39.62 d₂₀, d_(2m) (nm) = for d₂ < 18.21 37.46 80.09 126.81 27.34 d₂₀, d_(2m) (nm) =

TABLE 2-1 Case 2-06 2-07 2-08 2-09 2-10 n₁₀ 1.7803 1.7743 1.7445 1.7294 1.7425 k₁₀ 0.0868 0.0850 0.0789 0.0717 0.0762 d₁₀ (nm) 93.23 91.77 92.02 166.39 161.95 n₂₀ 1.9791 1.8636 1.7368 1.9163 1.9299 k₂₀ 0.3951 0.2810 0.2206 0.6369 0.3467 d₂₀ (nm) 77.05 139.87 212.33 26.72 78.23 for n₁ ≧ 1.8462 1.8349 1.8028 1.8016 1.8041 n₁₀, n_(1m) = for n₁ < 1.7475 1.7473 1.7193 1.7039 1.7237 n₁₀, n_(1m) = for k₁ ≧ 0.1496 0.1408 0.1323 0.1330 0.1299 k₁₀, k_(1m) = for k₁ < 0.0394 0.0374 0.0301 0.0370 0.0455 k₁₀, k_(1m) = for d₁ ≧ 109.31 108.27 115.67 209.20 195.88 d₁₀, d_(1m) (nm) = for d₁ < 87.00 86.56 85.73 157.85 156.76 d₁₀, d_(1m) (nm) = for n₂ ≧ 2.1009 1.9987 1.8971 2.0476 2.0364 n₂₀, n_(2m) = for n₂ < 1.8504 1.7392 1.6175 1.7703 1.8051 n₂₀, n_(2m) = for k₂ ≧ 0.5318 0.4468 0.3623 0.7342 0.4294 k₂₀, k_(2m) = for k₂ < 0.2922 0.2015 0.1499 0.5070 0.2516 k₂₀, k_(2m) = for d₂ ≧ 85.43 ∞ ∞ 31.20 85.58 d₂₀, d_(2m) (nm) = for d₂ < 68.38 126.05 181.56 22.38 72.33 d₂₀, d_(2m) (nm) =

TABLE 2-3 Case 2-11 2-12 2-13 2-14 2-15 n₁₀ 1.7364 1.7194 1.7189 1.7279 1.7039 k₁₀ 0.0767 0.0663 0.0609 0.0714 0.0620 d₁₀ (nm) 160.57 160.35 240.33 230.11 268.01 n₂₀ 1.7865 1.6960 2.2401 1.8887 1.7359 k₂₀ 0.2463 0.1988 0.7138 0.3299 0.2398 d₂₀ (nm) 145.39 214.32 17.92 78.86 158.55 for n₁ ≧ 1.7918 1.7729 1.7932 1.7879 1.7579 n₁₀, n_(1m) = for n₁ < 1.7262 1.6947 1.6903 1.7176 1.6407 n₁₀, n_(1m) = for k₁ ≧ 0.1172 0.1176 0.1266 0.1177 0.1322 k₁₀, k_(1m) = for k₁ < 0.0534 0.0312 0.0317 0.0558 0.0228 k₁₀, k_(1m) = for d₁ ≧ 198.97 ∞ ∞ ∞ ∞ d₁₀, d_(1m) (nm) = for d₁ < 157.73 149.13 225.89 226.73 223.91 d₁₀, d_(1m) (nm) = for n₂ ≧ 1.8969 1.9046 2.4255 2.0020 1.9149 n₂₀, n_(2m) = for n₂ < 1.6706 1.5895 2.0733 1.8277 1.4543 n₂₀, n_(2m) = for k₂ ≧ 0.3435 0.2910 0.8416 0.3876 0.4261 k₂₀, k_(2m) = for k₂ < 0.1729 0.1351 0.5371 0.2258 0.1424 k₂₀, k_(2m) = for d₂ ≧ 161.62 ∞ 21.50 87.70 ∞ d₂₀, d_(2m) (nm) = for d₂ < 139.39 187.96 15.15 76.00 129.53 d₂₀, d_(2m) (nm) =

TABLE 2-4 Case 2-4 n₁₀ 1.7046 k₁₀ 0.0595 d₁₀ (nm) 264.54 n₂₀ 1.7170 k₂₀ 0.1955 d₂₀ (nm) 223.28 for n₁ ≧ 1.7716 n₁₀, n_(1m) = for n₁ < 1.6465 n₁₀, n_(1m) = for k₁ ≧ 0.1321 k₁₀, k_(1m) = for k₁ < 0.0178 k₁₀, k_(1m) = for d₁ ≧ ∞ d₁₀, d_(1m) (nm) = for d₁ < 160.48 d₁₀, d_(1m) (nm) = for n₂ ≧ 2.1001 n₂₀, n_(2m) = for n₂ < 1.4760 n₂₀, n_(2m) = for k₂ ≧ 0.4081 k₂₀, k_(2m) = for k₂ < 0.1085 k₂₀, k_(2m) = for d₂ ≧ ∞ d₂₀, d_(2m) (nm) = for d₂ < 143.86. d₂₀, d_(2m) (nm) =


5. The patterning method according to claim 4, wherein the film thickness d₁ of said upper layer satisfies d₁ ≦250, and the film thickness d₂ of said lower layer satisfies d₂ ≦250.
 6. The patterning method according to claim 4, wherein the resist layer has a refractive index of 1.60 to 1.80.
 7. A method for patterning a resist layer comprising the steps of: providing a silicon semiconductor substrate; providing a resist layer above the semiconductor substrate; providing an antireflection film between a surface of the silicon semiconductor substrate and said resist layer; and exposing the resist layer to a light having a wave length of 190 nm to 195 nm via a system having a numerical aperture of more than 1.1 but less than or equal to 1.2, wherein, said antireflection film includes an upper layer having a complex refractive index N₁ equal to n₁ -k₁i and a film thickness d₁, and a lower layer having a complex refractive index N₂ equal to n₂ -k₂i and a film thickness d₂, said upper layer and said lower layer configured such that, the values of n₁₀, k₁₀, d₁₀, n₂₀, k₂₀, d₂₀, n₁, k₁, d₁, n₂, k₂ and d₂ satisfy a Formula 1 {(n ₁-n₁₀)/(n _(1m)-n ₁₀)}²+{(k ₁-k ₁₀)/(k _(1m)-k ₁₀)}²+{(d ₁-d ₁₀)/(d _(1m)-d ₁₀)}²+{(n ₂-n ₂₀) /(n _(2m)-n ₂₀)}²+{(k ₂-k ₂₀)/(k _(2m)-k ₂₀)}²+{(d ₂-d ₂₀)/(d _(2m)-d ₂₀)}²≦1,   Formula 1: the values of n₁₀, k₁₀, d₁₀, n₂₀, k₂₀, d₂₀, n₁, k₁, d₁, n₂, k₂ and d₂ are defined by one of cases [3-01] to [3-04]in Tables 3-1 to 3-4, (a) a value of n_(1m) in the pertaining case is adopted based on a relationship in magnitude between n₁ and n₁₀; (b) a value of k_(1m) in the pertaining case is adopted based on a relationship in magnitude between k₁ and k₁₀; (c) a value of d_(1m) in the pertaining case is adopted based on a relationship in magnitude between d₁ and d₁₀; (d) a value of n_(2m) in the pertaining case is adopted based on a relationship in magnitude between n₂ and n₂; (e) a value of k_(2m) in the pertaining case is adopted based on a relationship in magnitude between k₂ and k₂₀; and (f) a value of d_(2m) in the pertaining case is adopted based on a relationship in magnitude between d₂ and d₂₀, and Tables 4-1 through 4-4 are: TABLE 4-1 Case 3-01 3-02 3-03 3-04 3-05 n₁₀ 2.1010 1.9972 1.8971 1.8903 1.7614 k₁₀ 0.0000 0.1417 0.0932 0.1047 0.0933 d₁₀ (nm) 18.86 29.97 20.09 13.40 99.78 n₂₀ 2.3980 3.9849 1.8912 1.7190 1.8773 k₂₀ 0.9577 0.5156 0.3589 0.2691 0.6361 d₂₀ (nm) 20.51 29.99 144.86 225.69 29.70 for n₁ ≧ 2.1902 2.0806 1.9757 1.9938 1.8213 n₁₀, n_(1m) = for n₁ < 2.0333 1.9400 1.8442 1.8243 1.7445 n₁₀, n_(1m) = for k₁ ≧ 0.0791 0.2081 0.1538 0.1917 0.1313 k₁₀, k_(1m) = for k₁ < 0.0000 0.0680 0.0073 0.0023 0.0538 k₁₀, k_(1m) = for d₁ ≧ 22.17 34.24 27.46 20.29 118.37 d₁₀, d_(1m) (nm) = for d₁ < 16.20 26.95 16.03 9.40 96.05 d₁₀, d_(1m) (nm) = for n₂ ≧ 2.5150 4.1060 2.0062 1.8367 1.9517 n₂₀, n_(2m) = for n₂ < 2.2758 3.8579 1.7470 1.5737 1.7548 n₂₀, n_(2m) = for k₂ ≧ 1.0902 0.6644 0.5181 0.3688 0.7101 k₂₀, k_(2m) = for k₂ < 0.8269 0.4039 0.2637 0.1833 0.5274 k₂₀, k_(2m) = for d₂ ≧ 23.39 31.19 ∞ ∞ 33.13 d₂₀, d_(2m) (nm) = for d₂ < 17.92 28.87 85.53 141.88 25.36 d₂₀, d_(2m) (nm) =

TABLE 4-2 Case 3-06 3-07 3-08 3-09 3-10 n₁₀ 1.7825 1.7569 1.7277 1.7272 1.7147 k₁₀ 0.0898 0.0868 0.0740 0.0744 0.0633 d₁₀ (nm) 97.07 96.31 94.69 178.89 164.15 n₂₀ 2.0041 1.7847 1.6779 2.1865 1.6838 k₂₀ 0.3750 0.2610 0.2014 0.6947 0.1862 d₂₀ (nm) 75.78 148.77 220.98 19.20 215.48 for n₁ ≧ 1.8327 1.7995 1.7711 1.7845 1.7573 n₁₀, n_(1m) = for n₁ < 1.7698 1.7544 1.7097 1.7167 1.6822 n₁₀, n_(1m) = for k₁ ≧ 0.1223 0.0982 0.1152 0.1077 0.1011 k₁₀, k_(1m) = for k₁ < 0.0533 0.0642 0.0321 0.0488 0.0264 k₁₀, k_(1m) = for d₁ ≧ 109.28 111.91 114.36 218.45 ∞ d₁₀, d_(1m) (nm) = for d₁ < 94.62 95.76 89.11 175.03 147.22 d₁₀, d_(1m) (nm) = for n₂ ≧ 2.0899 1.8293 1.7201 2.2837 1.7321 n₂₀, n_(2m) = for n₂ < 1.9035 1.6980 1.5934 2.0604 1.6046 n₂₀, n_(2m) = for k₂ ≧ 0.4366 0.3015 0.2464 0.7527 0.2137 k₂₀, k_(2m) = for k₂ < 0.2899 0.2021 0.1479 0.5549 0.1380 k₂₀, k_(2m) = for d₂ ≧ 81.59 161.61 ∞ 21.11 235.37 d₂₀, d_(2m) (nm) = for d₂ < 70.00 146.51 196.47 16.79 195.03 d₂₀, d_(2m) (nm) =

TABLE 4-3 Case 3-11 3-12 3-13 3-14 n₁₀ 1.7036 1.7000 1.7012 1.7028 k₁₀ 0.0666 0.0723 0.0708 0.0661 d₁₀ (nm) 228.90 216.03 209.55 205.70 n₂₀ 2.1518 1.7881 1.7244 1.7099 k₂₀ 0.6409 0.3189 0.2345 0.1906 d₂₀ (nm) 21.01 93.79 164.15 230.44 for n₁ ≧ 1.7333 1.7203 1.7336 1.7514 n₁₀, n_(1m) = for n₁ < 1.6243 1.6387 1.6472 1.6539 n₁₀, n_(1m) = for k₁ ≧ 0.1086 0.1103 0.1181 0.1191 k₁₀, k_(1m) = for k₁ < 0.0356 0.0460 0.0368 0.0268 k₁₀, k_(1m) = for d₁ ≧ ∞ 227.26 237.88 ∞ d₁₀, d_(1m) (nm) = for d₁ < 181.97 190.09 179.63 173.04 d₁₀, d_(1m) (nm) = for n₂ ≧ 2.3031 1.9012 1.8497 1.8964 n₂₀, n_(2m) = for n₂ < 2.0795 1.7532 1.6568 1.5385 n₂₀, n_(2m) = for k₂ ≧ 0.7063 0.3281 0.3333 0.3179 k₂₀, k_(2m) = for k₂ < 0.5137 0.2264 0.1529 0.1170 k₂₀, k_(2m) = for d₂ ≧ 24.52 111.38 ∞ ∞ d₂₀, d_(2m) (nm) = for d₂ < 19.07 89.55 150.63 157.43. d₂₀, d_(2m) (nm) =


8. The patterning method according to claim 7, wherein the film thickness d₁ of said upper layer satisfies d₁ ≦250, and the film thickness d₂ of said lower layer satisfies d₂ ≦250.
 9. The patterning method according to claim 7, wherein the resist layer has a refractive index of 1.60 to 1.80.
 10. A method for patterning a resist layer comprising: the steps of: providing a silicon semiconductor substrate; providing a resist layer above the semiconductor substrate; providing an antireflection film between a surface of the silicon semiconductor substrate and said resist layer; and exposing the resist layer to light having a wavelength of 190 nm to 195 nm via a system having a numerical aperture of more than 1.2 but less than or equal to 1.3, wherein, said antireflection film includes an upper layer having a complex refractive index N₁ equal to n₁ -k₁i and a film thickness d₁, and a lower layer having a complex refractive index N₂ equal to n₂ -k₂i and a film thickness d₂, said upper layer and said lower layer configured such that n₁₀, k₁₀, d₁₀, n₂₀, k₂₀, d₂₀, n₁, k₁, d₁, n₂, k₂ and d₂ satisfy a Formula 1 {(n ₁-n ₁₀)/(n _(1m)-n ₁₀)}²+{(k ₁-k ₁₀)/(k _(1m)-k ₁₀)}²+{(d ₁-d ₁₀)/(d _(1m)-d ₁₀)}²+{(n ₂-n ₂₀) /(n _(2m)-n ₂₀)}²+{(k ₂-k ₂₀)/(k _(2m)-k ₂₀)}²+{(d ₂-d ₂₀)/(d _(2m)-d ₂₀)}² ≦1,   Formula 1: the values of n₁₀, k₁₀, d₁₀, n₂₀, k₂₀, d₂₀, n₁, k₁, d₁, n₂, k₂ and d₂ are defined by one of cases [4-01] to [4-10] in Tables 4-1 through 4-2, (a) a value of n_(1m) in the pertaining case is adopted based on a relationship in magnitude between n₁ and n₁₀; (b) a value of k_(1m) in the pertaining case is adopted based on a relationship in magnitude between k₁ and k₁₀; (c) a value of d_(1m) in the pertaining case is adopted based on a relationship in magnitude between d₁ and d₁₀; (d) a value of n_(2m) in the pertaining case is adopted based on a relationship in magnitude between n₂ and n₂₀; (e) a value of k_(2m) in the pertaining case is adopted based on a relationship in magnitude between k₂ and k₂₀; and (f) a value of d_(2m) in the pertaining case is adopted based on a relationship in magnitude between d₂ and d₂₀, and Tables 4-1 through 4-4 are: TABLE 4-1 Case 4-01 4-02 4-03 4-04 4-05 n₁₀ 2.0750 2.0118 1.8885 1.8806 1.7567 k₁₀ 0.0000 0.1190 0.0999 0.1003 0.0923 d₁₀ (nm) 20.30 29.87 17.71 13.44 108.92 n₂₀ 2.4310 4.0092 1.7811 1.7062 2.0485 k₂₀ 0.9366 0.5022 0.3211 0.2477 0.6631 d₂₀ (nm) 19.90 29.99 159.56 227.84 23.68 for n₁ ≧ 2.1541 2.0844 1.9589 1.9713 1.7997 n₁₀, n_(1m) = for n₁ < 2.0215 1.9638 1.8538 1.8291 1.7557 n₁₀, n_(1m) = for k₁ ≧ 0.0610 0.1705 0.1459 0.1729 0.0954 k₁₀, k_(1m) = for k₁ < 0.0000 0.0518 0.0187 0.0078 0.0655 k₁₀, k_(1m) = for d₁ ≧ 23.54 33.58 23.82 19.76 125.01 d₁₀, d_(1m)(nm) = for d₁ < 18.03 27.42 15.13 10.09 108.67 d₁₀, d_(1m)(nm) = for n₂ ≧ 2.5291 4.1084 1.8635 1.7809 2.0547 n₂₀, n_(2m)= for n₂ < 2.3203 3.9019 1.6624 1.5899 1.9572 n₂₀, n_(2m)= for k₂ ≧ 1.0610 0.6325 0.4092 0.3139 0.6691 k₂₀, k_(2m)= for k₂ < 0.8178 0.4040 0.2433 0.1176 0.5710 k₂₀, k_(2m)= for d₂ ≧ 22.43 30.97 ∞ ∞ 23.86 d₂₀, d_(2m)(nm) = for d₂ < 17.62 29.03 129.86 149.42 21.22 d₂₀, d_(2m)(nm) =

TABLE 4-2 Case 4-06 4-07 4-08 4-09 4-10 n₁₀ 1.7300 1.7016 1.7036 1.7088 1.7083 k₁₀ 0.0690 0.0665 0.0722 0.0700 0.0641 d₁₀ (nm) 99.33 227.28 216.05 208.98 205.66 n₂₀ 1.7059 2.1201 1.7959 1.7311 1.7076 k₂₀ 0.1911 0.6392 0.3181 0.2343 0.1900 d₂₀ (nm) 215.34 21.82 93.13 163.14 228.20 for n₁ ≧ 1.7599 1.7325 1.7213 1.7343 1.7487 n₁₀, n_(1m) = for n₁ < 1.7290 1.6697 1.6816 1.6905 1.6839 n₁₀, n_(1m) = for k₁ ≧ 0.0744 0.1071 0.1083 0.1002 0.0965 k₁₀, k_(1m) = for k₁ < 0.0522 0.0350 0.0475 0.0408 0.0326 k₁₀, k_(1m) = for d₁ ≧ 114.51 249.66 226.44 234.14 ∞ d₁₀, d_(1m) (nm) = for d₁ < 98.99 206.91 203.38 198.02 187.04 d₁₀, d_(1m) (nm) = for n₂ ≧ 1.7114 2.2630 1.9107 1.8583 1.8700 n₂₀, n_(2m) = for n₂ < 1.6501 2.0448 1.7644 1.6757 1.5497 n₂₀, n_(2m) = for k₂ ≧ 0.1929 0.7020 0.3809 0.3287 0.3066 k₂₀, k_(2m) = for k₂ < 0.1524 0.5119 0.2256 0.1573 0.1188 k₂₀, k_(2m) = for d₂ ≧ 219.55 25.26 110.64 ∞ ∞ d₂₀, d_(2m) (nm) = for d₂ < 205.88 19.68 89.45 150.12 160.78. d₂₀, d_(2m) (nm) =


11. The patterning method according to claim 10, wherein the film thickness d₁ of said upper layer satisfies d₁ ≦250, and the film thickness d₂ of said lower layer satisfies d₂ ≦250.
 12. The patterning method according to claim 10, wherein the resist layer has a refractive index of 1.60 to 1.80.
 13. A method for patterning a resist layer comprising the steps of: providing silicon semiconductor substrate; providing a resist layer above the semiconductor substrate; providing an antireflection film between a surface of the silicon semiconductor substrate and said resist layer; and exposing the resist layer to light having a wave length of 190 nm to 195 nm via a system having a numerical aperture of more than 1.3 but less than or equal to 1.4, wherein, said antireflection film includes an upper layer having a complex refractive index N₁ equal to n₁-k₁i and a film thickness d₁, and a lower layer having a complex refractive index N₂ equal to n₂-k₂i and a film thickness d₂, said upper layer and said lower layer configured such that the values of n₁₀, k₁₀, d₁₀, n₂₀, k₂₀, d₂₀, n₁, k₁, d₁, n₂, k₂ and d₂ satisfy a Formula 1 {(n ₁-n ₁₀)/(n _(1m)-n ₁₀)}²+{(k ₁-k ₁₀)/(k _(1m)-k ₁₀)}²+{(d ₁-d ₁₀)/(d _(1m)-d ₁₀)}²+{(n ₂-n ₂₀) /(n _(2m)-n ₂₀)}²+{(k ₂-k ₂₀)/(k _(2m)-k ₂₀)}²+{(d ₂-d ₂₀)/(d _(2m)-d ₂₀)}²≦1,   Formula 1: the values of n₁₀, k₁₀, d₁₀, n₂₀, k₂₀, d₂₀, n₁, k₁, d₁, n₂, k₂ and d₂ are defined by on of cases [5-01] to[5-07] in Table 5-1 through 5-2, (a) a value of n_(1m) in the pertaining case is adopted based on a relationship in magnitude between n₁ and n₁₀; (b) a value of k_(1m) in the pertaining case is adopted based on a relationship in magnitude between k₁ and k₁₀; (c) a value of d_(1m) in the pertaining case is adopted based on a relationship in magnitude between d₁ and d₁₀; a value of n_(2m) in the pertaining case is adopted based on a relationship in magnitude between n₂ and n₂₀; (e) a value of k_(2m) in the pertaining case is adopted based on a relationship in magnitude between k₂ and k₂₀; and (f) a value of d_(2m) in the pertaining case is adopted based on a relationship in magnitude between d₂ and d₂₀, and Tables 5-1 through 5-4 are: TABLE 5-1 Case 5-01 5-02 5-03 5-04 5-05 n₁₀ 2.0901 2.0375 1.8787 1.8780 1.7009 k₁₀ 0.0000 0.0819 0.1028 0.0706 0.0609 d₁₀ (nm) 20.79 29.12 16.60 14.89 160.18 n₂₀ 2.4315 3.6552 1.7172 1.7467 1.6995 k₂₀ 0.9254 0.4960 0.2840 0.2361 0.1745 d₂₀ (nm) 20.34 34.09 167.85 221.06 215.71 for n₁ ≧ 2.1532 2.0916 1.9323 1.9461 1.7131 n₁₀, n_(1m) = for n₁ < 2.0485 1.9946 1.8625 1.8482 1.6965 n₁₀, n_(1m) = for k₁ ≧ 0.0301 0.1157 0.1287 0.1125 0.0797 k₁₀, k_(1m) = for k₁ < 0.0000 0.0234 0.0358 0.0000 0.0529 k₁₀, k_(1m) = for d₁ ≧ 23.53 31.97 21.01 20.40 168.49 d₁₀, d_(1m) (nm) = for d₁ < 19.45 27.24 15.35 12.65 156.71 d₁₀, d_(1m) (nm) = for n₂ ≧ 2.4915 3.7301 1.7470 1.7894 1.7056 n₂₀, n_(2m) = for n₂ < 2.3369 3.5977 1.6335 1.6492 1.6786 n₂₀, n_(2m) = for k₂ ≧ 1.0253 0.5706 0.3145 0.2771 0.1981 k₂₀, k_(2m) = for k₂ < 0.8408 0.4125 0.2297 0.1801 0.1502 k₂₀, k_(2m) = for d₂ ≧ 22.48 35.05 ∞ ∞ 219.96 d₂₀, d_(2m) (nm) = for d₂ < 18.31 33.41 144.47 152.04 200.15 d₂₀, d_(2m) (nm) =

TABLE 5-2 Case 5-06 5-07 n₁₀ 1.7204 1.7142 k₁₀ 0.0677 0.0552 d₁₀ (nm) 231.66 225.66 n₂₀ 2.2460 1.7026 k₂₀ 0.6523 0.1831 d₂₀ (nm) 18.88 210.32 for n₁ ≧ 1.7346 1.7449 n₁₀, n_(1m) = for n₁ < 1.7142 1.7015 n₁₀, n_(1m) = for k₁ ≧ 0.0791 0.0776 k₁₀, k_(1m) = for k₁ < 0.0480 0.0279 k₁₀, k_(1m) = for d₁ ≧ 241.66 269.84 d₁₀, d_(1m) (nm) = for d₁ < 227.75 215.83 d₁₀, d_(1m) (nm) = for n₂ ≧ 2.3315 1.8141 n₂₀, n_(2m) = for n₂ < 2.2068 1.6257 n₂₀, n_(2m) = for k₂ ≧ 0.6941 0.2591 k₂₀, k_(2m) = for k₂ < 0.5188 0.1258 k₂₀, k_(2m) = for d₂ ≧ 20.91 ∞ d₂₀, d_(2m) (nm) = for d₂ < 17.96 186.01. d₂₀, d_(2m) (nm) =


14. The patterning method according to claim 13, wherein the film thickness d₁ of said upper layer satisfies d₁ ≦250, and the film thickness d₂ of said lower layer satisfies d₂ ≦250.
 15. The patterning method according to claim 13, wherein the resist layer has a refractive index of 1.60 to 1.80. 